Spectroscopic Studies of Dioxygen-Activating Functional Heme Models

• Project/Area Number: 21750064
• Research Category: Grant-in-Aid for Young Scientists (B)
• Allocation Type: Single-year Grants
• Research Field: Inorganic chemistry
• Research Institution: Kyushu University
• Principal Investigator: OHTA Takehiro 九州大学, 先導物質化学研究所, 助教 (70509950)
• Co-Investigator(Renkei-kenkyūsha): NARUTA Yoshinori 九州大学, 先導物質化学研究所, 教授 (00108979) ; LIU Jin-gang 九州大学, 先導物質化学研究所教授, 特任准 (70380540)
• Project Period (FY): 2009 – 2011
• Project Status: Completed (Fiscal Year 2011)
• Budget Amount: ¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000); Fiscal Year 2011: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000); Fiscal Year 2010: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000); Fiscal Year 2009: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
• Keywords: ポルフィリン / モデル化 / 共鳴ラマン分光 / 分子触媒化学 / 生物無機化学 / 酸素活性化 / 量子化学計算 / 金属酵素 / 分子触媒 / 振動分光学 / 生体模倣触媒 / 核共鳴非弾性散乱分光

Research Abstract

The dioxygen activation catalyzed by metallenzymes is important chemistry in terms of development of energy conversion catalysts. Elucidation of the dioxygen activation mechanism is highly desired to understand the design principle of the nature for the development of bio-inspired molecular catalysts. Thus functional heme models are used for the investigation of the dioxygen activation mechanism applying spectroscopic methods, providing fundamental insights into the biological mechanism which underlies the efficacy of the catalyst.

Research Products

• [Journal Article] Cytochrome C552 from Thermus thermophilus Engineered for Facile Substitution of Prosthetic Group (2011)
  • Author(s): S. M. Ibrahim, H. Nakajima, T. Ohta, K. Ramanathan, N. Takatani, Y. Naruta, Y. Watanabe
  • Journal Title: Biochemistry Volume: 50 Pages: 9826-9835
  • Peer Reviewed
• [Journal Article] Cytochrome c552 from Thermus Thermophilus Engineered for Facile Substitution of Prosthetic Group (2011)
  • Author(s): Sk. Md. Ibrahim, H. Nakajima, K. Ramanathan, N. Takatani, T. Ohta, Y. Naruta, Y. Watanabe
  • Journal Title: Biochemistry Volume: 50(45) Issue: 45 Pages: 9826-9835
  • DOI: 10.1021/bi201048e
  • Peer Reviewed
• [Journal Article] Formation of an End-On Ferric Peroxo Intermediate upon One-Electron Reduction of a Ferric Superoxo Heme (2010)
  • Author(s): J.-G. Liu, Y. Shimizu, T. Ohta, Y. Naruta
  • Journal Title: J. Am. Chem. Soc Volume: 132 Pages: 3672-3673
  • Peer Reviewed
• [Journal Article] Oxoferryl Porphyrin/Hydrogen Peroxide System Whose Behavior is Equivalent to Hydroperoxoferric Porphyrin (2010)
  • Author(s): H.Kitagishi, M.Tamaki., T.Ueda, S.Hirota, T.Ohta, Y.Naruta, K.Kano
  • Journal Title: J.Am.Chem.Soc. Volume: 132 Pages: 16730-1673
  • Peer Reviewed
• [Journal Article] Formation of an End-on Ferric-Peroxo Intermediate upon One-Electron Reduction of a Ferric-Superoxo Heme (2010)
  • Author(s): J.-G.Liu, Y.Shimizu, T.Ohta, Y.Naruta
  • Journal Title: The Journal of the American Chemical Society 132 Pages: 3672-3673
  • Peer Reviewed
• [Journal Article] Angew. Chem (2009)
  • Author(s): J.-G. Liu, T. Ohta, Y. Yamaguchi, T. Ogura, S. Sakamoto, Y. Maeda, Y. Naruta
  • Journal Title: Int. Ed Volume: 48 Pages: 9262-9267
  • Peer Reviewed
• [Journal Article] Synthesis and Characterization of a New Prostaglandin H Synthase Model (2009)
  • Author(s): J. J. Reddy, T. Ohta, Y. Naruta
  • Journal Title: Tetrahedron Letters Volume: 50 Pages: 3418-3421
  • Peer Reviewed
• [Journal Article] Spectroscopic Characterization of a Hydroperoxo-Heme Intermediate of a Synthetic Model : Conversion of a Side-on Peroxy to an End-on Hydroperoxy Complex (2009)
  • Author(s): J.-G.Liu, T.Ohta, S.Yamaguchi, T.Ogura, S.Sakamoto, Y.Maeda, Y.Naruta
  • Journal Title: Angewandte Chemie International Edition 48 Pages: 9262-9267
  • Peer Reviewed
• [Journal Article] Synthesis and Characterization of a New Prostaglandin H Synthase Model (2009)
  • Author(s): J.J.Reddy, T.Ohta, Y.Naruta
  • Journal Title: Tetrahedron Letters 50 Pages: 3418-3421
  • Peer Reviewed
• [Journal Article] Resonance Raman Characterization of Mononuclear Heme-Peroxo Intermediate Models
  • Author(s): T. Ohta, J-. G. Liu, Y. Naruta
  • Journal Title: Coord. Chem. Rev Volume: (印刷中)
  • Peer Reviewed
• [Presentation] Spectroscopic Insights into the Molecular Mechanism of Dioxygen Activation by Functional Heme Models (2012)
  • Author(s): T. Ohta, J-. G. Liu, P. Nagaraju, Y. Naruta
  • Organizer: 243rd American Chemical Society National Meeting
  • Place of Presentation: San Diego, USA(Invited talk)
  • Year and Date: 2012-03-27
• [Presentation] Spectroscopic Insights into the Molecular Mechanism of Dioxygen Activation by Functional Heme Models (2012)
  • Author(s): T.Ohta, J-.G.Liu, P.Nagaraju, Y.Naruta
  • Organizer: 243^<rd> American Chemical Society National Meeting
  • Place of Presentation: San Diego Convention Center, USA(招待講演)
  • Year and Date: 2012-03-27
• [Presentation] 酸素活性化ヘム酵素モデル錯体の分光学的研究 (2011)
  • Author(s): 太田雄大,劉勁剛,依田芳卓,斎藤真器名,小林康浩,瀬戸誠,成田吉徳
  • Organizer: 第44回酸化反応討論会
  • Place of Presentation: 大阪
  • Year and Date: 2011-11-04
• [Presentation] 酸素活性化ヘム酵素モデル錯体の分光学的研究 (2011)
  • Author(s): 太田雄大, 劉勁剛, 依田芳卓, 斎藤真器名, 小林康浩, 瀬戸誠, 成田吉徳
  • Organizer: 第44回酸化反応討論会
  • Place of Presentation: 大阪大学,大阪
  • Year and Date: 2011-11-04
• [Presentation] 酸素活性化ヘム酵素モデル錯体の分光学的研究 (2011)
  • Author(s): 太田雄大,劉勁剛,依田芳卓,斎藤真器名,小林康浩,瀬戸誠,成田吉徳
  • Organizer: 第61回錯体化学討会
  • Place of Presentation: 岡山
  • Year and Date: 2011-09-17
• [Presentation] 酸素活性化ヘム酵素モデル錯体の分光学的研究 (2011)
  • Author(s): 太田雄大, 劉勁剛, 依田芳卓, 斎藤真器名, 小林康浩, 瀬戸誠, 成田吉徳
  • Organizer: 第61回錯体化学討会
  • Place of Presentation: 岡山理科大学,岡山
  • Year and Date: 2011-09-17
• [Presentation] NRVS and DFT Analyses of Heme-Peroxy Adducts (2011)
  • Author(s): T. Ohta, J.-G. Liu, P. Nagaraju, Y. Naruta
  • Organizer: International Symposium on Activation of Dioxygen and Homogeneous Catalytic Oxidation
  • Place of Presentation: Okinawa(Oral presentation)
  • Year and Date: 2011-07-08
• [Presentation] NRVS and DFT Analyses of Heme-Peroxy Adducts (2011)
  • Author(s): T.Ohta. J.-G.Liu, P.Nagaraiu, Y.Naruta
  • Organizer: International Symposium on Activation of Dioxygen and Homogeneous Catalytic Oxidation
  • Place of Presentation: Bankoku Shinryokan, Okinawa
  • Year and Date: 2011-07-08
• [Presentation] Spectroscopic and Computational Studies of Oxygen-activating Functional Heme Models (2011)
  • Author(s): T. Ohta, J-. G. Liu, M. Saito, Y. Kobayashi, Y. Yoda, Y. Naruta, M. Seto
  • Organizer: The International Symposium on Molecular Systems, Global COE Symposium for Young Researchers
  • Place of Presentation: Fukuoka(Oralpresentation)
  • Year and Date: 2011-05-11
• [Presentation] Spectroscopic and Computational Studies of Oxygen-activating Functional Heme Models (2011)
  • Author(s): T.Ohta. J-.G.Liu, M.Saito, Y.Kobayashi, Y.Yoda, Y.Naruta, M.Seto
  • Organizer: The International Symposium on Molecular Systems, Global COE Symposium for Young Researchers
  • Place of Presentation: The Luigans, Fukuoka
  • Year and Date: 2011-05-11
• [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: 2011-03-26
• [Presentation] 捕捉困難なヘム-ニトロキシル錯体の合成と分光学的同定 (2011)
  • Author(s): 劉勁剛, 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: 2011-03-26
• [Presentation] 酸素還元のためのBio-inspired分子触媒の合成 (2011)
  • Author(s): P.Nagaraju, 劉勁剛, 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: 2011-03-26
• [Presentation] Bio-inspired Model Compounds for Oxygen Activation and Reduction (2011)
  • Author(s): 劉勁剛, 太田雄大, 成田吉徳
  • Organizer: 九州大学I2CNERワークショップ
  • Place of Presentation: 福岡
  • Year and Date: 2011-02-04
• [Presentation] Solution Capturing End-On Peroxo and Hydroperoxo Intermediates of Heme Enzymes (2010)
  • Author(s): 劉勁剛, 太田雄大, 清水雄太, 成田吉徳
  • Organizer: 環太平洋国際化学会議2010
  • Place of Presentation: ホノルル(米国)
  • Year and Date: 2010-12-19
• [Presentation] Activation and catalytic reduction of dioxygen : Lessons from heme enzyme chemical models (2010)
  • Author(s): 成田吉徳, 劉勁剛, 太田雄大, A.C.Maity, 清水雄太, 谷文都
  • Organizer: 環太平洋国際化学会議2010
  • Place of Presentation: ホノルル(米国)
  • 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] 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 Models (2010)
  • Author(s): 劉勁剛, 太田雄大, 成田吉徳
  • Organizer: 60th Anniversary Conference on Coordination Chemistry_Chem.Commun.Symposium
  • Place of Presentation: 大阪
  • Year and Date: 2010-09-28
• [Presentation] Efficient Electrocatalytic Water Oxidation with Manganese and Cobalt Porphyrin Dimers-ITO Assembly (2010)
  • 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] 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] 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徳 (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: 近畿大学(大阪府)
  • 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: 近畿大学(大阪府)
  • 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: 近畿大学(大阪府)
  • Year and Date: 2010-03-28
• [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 (2010)
  • Author(s): 劉勁剛・太田雄大・清水雄太・成田吉徳
  • Organizer: 日本化学会第90春季年会
  • Place of Presentation: 近畿大学(大阪府)
  • 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徳 (2010)
  • Author(s): Zahran, Zaki・太坦雄大・王昂・成田吉徳
  • Organizer: 日本化学会第90春季年会
  • Place of Presentation: 近畿大学(大阪府)
  • 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): Reddy, Jakkidi・太田雄大・成田吉徳
  • Organizer: 日本化学会第90春季年会
  • Place of Presentation: 近畿大学(大阪府)
  • Year and Date: 2010-03-26
• [Presentation] Mn-Porphyrin as a New Prostaglandin H Synthase Model : Its Catalytic Oxygenation of All-cis-Polyenes (2010)
  • 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
  • Year and Date: 2009-11-19
• [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: 京都大学(京都府宇治市)
  • Year and Date: 2009-11-19
• [Presentation] Efficient Electrolytic Water Oxidation with Manganese Porphyrin Dimer Catalysts Assembled on ITO Electrodes (2009)
  • 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: 東北大学(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: 東北大学(仙台)
  • Year and Date: 2009-11-15
• [Presentation] β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: 長崎大学(長崎県長崎市)
  • Year and Date: 2009-09-26
• [Presentation] Synthetic heme models to mimic the formation of ferric peroxo and hydroperoxo intermediates involved in heme-containing enzymes (2009)
  • Author(s): 劉勁剛・太田雄大・清水雄太・成田吉徳
  • Organizer: 第59回錯体化学討論会
  • Place of Presentation: 長崎大学(長崎県長崎市)
  • 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: 長崎大学(長崎県長崎市)
  • Year and Date: 2009-09-25
• [Presentation] Mn-Porphyrin models of prostaglandin H synthases and their catalytic oxygenation of all-cis-polyenes (2009)
  • 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: 九州大学(福岡)
  • Year and Date: 2009-09-15
• [Presentation] A novel dioxygen activation by a heme-copper binuclear complex (2009)
  • Author(s): T. Ohta, T. Chishiro, F. Tani and Y. Naruta
  • Organizer: 14th International Conference on Biological Inorganic Chemistry
  • Place of Presentation: Nagoya
  • Year and Date: 2009-07-27
• [Presentation] A novel dioxygen activation by a heme-copper binuclear complex (2009)
  • Author(s): T.Ohta, T.Chishiro, F.Tani, Y.Naruta
  • Organizer: 14th International Conference on Biological Inorganic Chemistry (ICBIC 14)
  • Place of Presentation: 名古屋国際会議場(愛知県)
  • Year and Date: 2009-07-27
• [Presentation] Preparation of Low-spin End-on Ferric-Peroxo and Ferric- Hydroperoxo Species by a Heme Model Complex Bearing an Imidazole Tail (2009)
  • Author(s): J.-G.Liu, T.Ohta, S.Yamaguchi, T.Ogura, Y.Naruta
  • Organizer: 14th International Conference on Biological Inorganic Chemistry (ICBIC 14)
  • Place of Presentation: 名古屋国際会議場(愛知県)
  • Year and Date: 2009-07-26
• [Remarks]
  • URL: http://hyoka.ofc.kyushu-u.ac.jp/search/details/K003730/index.html
• [Remarks]
  • URL: http://hyoka.ofc.kyushu-u.ac.jp/search/details/K003730/research.html