QM/MM study on the oxygen active species in metalloenzymes

• Project/Area Number: 18750048
• Research Category: Grant-in-Aid for Young Scientists (B)
• Allocation Type: Single-year Grants
• Research Field: Inorganic chemistry
• Research Institution: Kyushu University
• Principal Investigator: KAMACHI Takashi Kyushu University, 先導物質化学研究所, 学術研究員 (40403951)
• Project Period (FY): 2006 – 2008
• Project Status: Completed (Fiscal Year 2008)
• Budget Amount: ¥4,000,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥300,000); Fiscal Year 2008: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000); Fiscal Year 2007: ¥1,100,000 (Direct Cost: ¥1,100,000); Fiscal Year 2006: ¥1,600,000 (Direct Cost: ¥1,600,000)
• Keywords: 量子化学 / 酵素反応 / 遷移状態 / 金属酵素活性種 / 密度汎関数法 / QM / MM法 / MM 法

Research Abstract

本研究では量子化学計算を用いて、金属酵素活性種が有する特殊な電子状態や反応性を解析した。特にQM/MM法を用いた計算から、酵素全体の影響を考慮したより現実に近い検討を行った。これらの成果により、これまで9報が学術論文誌に掲載された。また、国内外の学会で積極的に発表を行い高い評価を得た。

Research Products

• [Journal Article] Bulletin of the Chemical Society of Japan (2008)
  • Author(s): T. Kamachi, T. Nakayama, K. Yoshizawa
  • Journal Title: BCSJ Award Article 81 Pages: 1212-1212
  • Peer Reviewed
• [Journal Article] The Journal of Physical Chemistry C (2008)
  • Author(s): A. Staykov, T. Kamachi, T. Ishihara, K. Yoshizawa
  • Journal Title: 112 Pages: 19501-19501
  • Peer Reviewed
• [Journal Article] The Journal of Physical Chemistry A (2008)
  • Author(s): T. Kamachi, Y.-M. Lee, T. Nishimi, J. Cho, K. Yoshizawa, W. Nam
  • Journal Title: 112 Pages: 13102-13102
  • Peer Reviewed
• [Journal Article] Mechanism and Kinetics of Cyanide Decomposition by Ferrate (2008)
  • Author(s): Kamachi, et.al.
  • Journal Title: Bulletin of the Chemical Society of Japan 81 Pages: 1212-1218
  • NAID: 10024330607
  • Peer Reviewed
• [Journal Article] Theoretical Study of the Direct Synthesis of H_2O_2 on Pd and Pd/Au Surfaces (2008)
  • Author(s): Staykov, et.al.
  • Journal Title: The Journal of Physical Chemistry C 112 Pages: 19501-19505
  • Peer Reviewed
• [Journal Article] Combined Experimental and Theoretical Approach to Understand the Reactivity of a Mononuclear Cu(II)-Hydroperoxo Complex in Oxygenation Reactions (2008)
  • Author(s): Kamachi, et.al.
  • Journal Title: The Journal of Physical Chemistry A 12 Pages: 13102-13108
  • Peer Reviewed
• [Journal Article] Angewandete Chemie International Edition (2007)
  • Author(s): P. M. Kozlowski, T. Kamachi, T. Toraya, K. Yoshizawa
  • Journal Title: 46 Pages: 980-980
  • Peer Reviewed
• [Journal Article] Angewandete Chemie International Edition (2007)
  • Author(s): M. S. Seo, T. Kamachi, T. Kouno, K. Murata, M. J. Park, K. Yoshizawa, W. Nam
  • Journal Title: 46 Pages: 2291-2291
  • Peer Reviewed
• [Journal Article] The Journal of Physical Chemistry A (2007)
  • Author(s): K. Yoshizawa, T. Nakayama, T. Kamachi, P. M. Kozlowski
  • Journal Title: 111 Pages: 852-852
  • Peer Reviewed
• [Journal Article] Chemistry - A European Journal (2007)
  • Author(s): T. Kamachi, T. Toraya, K. Yoshizawa
  • Journal Title: 13 Pages: 7864-7864
  • Peer Reviewed
• [Journal Article] Computational Mutation Analysis of Hydrogen Abstraction and Radical Rearrangement Steps in the Catalysis of Coenzyme B12-Dependent Diol Dehydratase (2007)
  • Author(s): Kamachi, et. al.
  • Journal Title: Chemisty A european Joumal 13 Pages: 7864-7873
  • Peer Reviewed
• [Journal Article] Experimental and Theoretical Evidence for Nonheme Iron(III)Alkylperoxo Species as Sluggish Oxidants in Oxygenation Reactions (2007)
  • Author(s): M.S., Seo, et. al.
  • Journal Title: Angewandete Chemie Intermational Edition 46 Pages: 2291-2294
  • Peer Reviewed
• [Journal Article] Vibronic Interaction in Metalloporphyrin π-Anion Radicals (2007)
  • Author(s): Yoshizawa, et. al.
  • Journal Title: Joumal of Physical Chemistry 111 Pages: 852-857
  • Peer Reviewed
• [Journal Article] Does Cob(II)alamin Act as a Conductor in Coenzyme B_<12> Dependent Mutases? (2007)
  • Author(s): P.M.Kozlowski et al.
  • Journal Title: Angewandete Chemie International Edition 46 Pages: 980-980
• [Journal Article] Experimental and Theoretical Evidence for Nonheme Iron(III) Alkylperoxo Species as Sluggish Oxidants in Oxygenation Reactions (2007)
  • Author(s): M.S.Seo et al.
  • Journal Title: Angewandete Chemie International Edition 46 Pages: 2291-2291
• [Journal Article] How Axial Ligands Control the Reactivity of High-Valent Iron(IV)-Oxo Porphyrin π-Cation Radicals in Alkane Hydroxylation : A Computational Study (2006)
  • Author(s): T.Kamachi et al.
  • Journal Title: Journal of Inorganic Biochemistry 100 Pages: 751-751
• [Journal Article] Catalytic Mechanism of Dopamine β-Monooxygenase Mediated by Cu(III)-Oxo (2006)
  • Author(s): K.Yoshizawa et al.
  • Journal Title: Inorganic Chemistry 45 Pages: 3034-3034
• [Journal Article] The Journal of Physical Chemistry B
  • Author(s): T. Kamachi, M. Takahata, T. Toraya, K. Yoshizawa
  • Journal Title: Journal Cover (in press)
  • Peer Reviewed
• [Journal Article] Chemistry - A European Journal
  • Author(s): T. Kamachi, T. Nakayama, O. Shitamichi, K. Jitsumori,T. Kurihara, N. Esaki, K. Yoshizawa
  • Journal Title: (in press)
  • Peer Reviewed
• [Presentation] ビタミンB12依存型酵素の反応性に関する理論的研究 (2009)
  • Author(s): 蒲池高志、Kozlowski Pawel、虎谷哲夫、吉澤一成
  • Organizer: 日本化学会第89春季年会
  • Place of Presentation: 船橋
  • Year and Date: 2009-03-27
• [Presentation] Theoretical Study on the Mechanism of Catalysis of Coenzyme B12-Dependent Glutamate Mutase (2008)
  • Author(s): T. Kamachi, P. M. Kozlowski, T. Toraya, K. Yoshizawa
  • Organizer: Asian Biological Inorganic Chemistry Conference 4th
  • Place of Presentation: Jeju
  • Year and Date: 2008-11-10
• [Presentation] Theoretical Study on the Mechanism of Catalysis of Coenzyme B_<12>-Dependent Glutamate Mutase (2008)
  • Author(s): Kamachi, et.al.
  • Organizer: Asian Biological Inorganic Chemistry Conference 4th
  • Place of Presentation: 済州島韓国
  • Year and Date: 2008-11-10
• [Presentation] ビタミンB12依存型酵素の反応機構に関する理論的研究 (2008)
  • Author(s): 蒲池高志、Kozlowski Pawel、虎谷哲夫、吉澤一成
  • Organizer: 分子科学討論会2008
  • Place of Presentation: 福岡
  • Year and Date: 2008-09-24
• [Presentation] アルキルペルオキソ鉄(III)錯体の反応性に関する理論的研究 (2008)
  • Author(s): 蒲池高志、村田幸司、向野智久、W. Nam、吉澤一成
  • Organizer: 日本化学会第88春季年会
  • Place of Presentation: 東京
  • Year and Date: 2008-03-26
• [Presentation] アルキルペルオキソ鉄(III)錯体の密度汎関数法による反応性解析 (2007)
  • Author(s): 蒲池高志、村田幸司、向野智久、W. Nam、吉澤一成
  • Organizer: 分子科学討論会2007
  • Place of Presentation: 仙台
  • Year and Date: 2007-09-17
• [Presentation] Stabilization of Substrate Radicals by Cob(II)alamin in Coenzyme B12 Dependent Mutase. An Instight form DFT Calculations (2007)
  • Author(s): T. Kamachi, P. M. Kozlowski, T. Toraya, K. Yoshizawa
  • Organizer: International Conference on Biological Inorganic Chemistry13th
  • Place of Presentation: Vienna
  • Year and Date: 2007-07-15
• [Presentation] ジオールデヒドラターゼ変異型酵素の反応性に関する理論的検討 (2007)
  • Author(s): 蒲池高志、虎谷哲夫、吉澤一成
  • Organizer: 日本化学会第87春季年会
  • Place of Presentation: 大阪
  • Year and Date: 2007-03-25
• [Presentation] Stabilization of Substrate Radicals by Cob(II)alamin in Coenzyme B12 Dependent Mutase. An Instinght form DFR Calculations (2007)
  • Author(s): Kamachi, et. al.
  • Organizer: International Conference on Biological Chemistry 13 th
  • Place of Presentation: ウーイン
• [Presentation] ジオールデヒドラターゼ変異型酵素の反応性に関する理論的解析 (2006)
  • Author(s): 蒲池高志、虎谷哲夫、吉澤一成
  • Organizer: 日本化学会西日本大会2006
  • Place of Presentation: 沖縄
  • Year and Date: 2006-11-18
• [Presentation] ジオールデヒドラターゼ変異型酵素の反応性に関する理論的解析 (2006)
  • Author(s): 蒲池高志、吉澤一成
  • Organizer: 第98回触媒討論会
  • Place of Presentation: 富山
  • Year and Date: 2006-09-26
• [Presentation] QM/MM法によるジオールデヒドラターゼ変異体の反応性解析 (2006)
  • Author(s): 蒲池高志、虎谷哲夫、吉澤一成
  • Organizer: 分子構造総合討論会2006
  • Place of Presentation: 静岡
  • Year and Date: 2006-09-20
• [Presentation] Theoretical Study on the Mechanism of Catalysis of Coenzyme B12-Dependent Diol Dehydratase (2006)
  • Author(s): Takashi Kamachi, Tetsuo Toraya, Kazunari, Yoshizawa
  • Organizer: EUROBIC 2006
  • Place of Presentation: Portugal
  • Year and Date: 2006-07-02
• [Presentation] Water-assisted oxo mechanism for heme metabolism (2006)
  • Author(s): Takashi Kamachi and Kazunari, Yoshizawa
  • Organizer: XIIth International Congress of Quantum Chemistry
  • Place of Presentation: Kyoto
  • Year and Date: 2006-05-21