Mechanism of Superoxide Dismutase-Like Activity of Fe(II) and Fe(III) Complexes of Tetrakis-N, N, N', N' (2-pyridylmethyl)ethylenediamine

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概要

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• The superoxide dismutase (SOD) activity of iron(II) tetrakis-N, N, N', N' (2-pyridylmethyl)ethylenediamine complex (Fe-TPEN) was reexamined using a pulse radiolysis mehtod. In our previous study (J. Biol. Chem., 264,9243-9249 (1989)), we reportd that this complex has a potent SOD activity in a cyt. c (cytochrome c)-based system (IC_<50>=0.8 μM) and protects E. coli cells against paraquat toxicity . The present pulse radiolysis experiment revealed that Fe(II)TPEN reacts stoichiometrically with superoxide to form Fe(III)TPEN with a second-order rate constant of 3.9×10^6M^<-1>s^<-1> at pH 7.1,but superoxide did not reduce Fe(III)TPEN to Fe(II)TPEN. The reaction of Fe(III)TPEN and superoxide was biphasic. In the fast reaction, an adduct (Fe(III)TPEN-superoxide complex) was formed at the second-order rate constant of 8.5×10^5_M^<-1>_S^<-1> at pH 7.4. In the slow one, the adduct reacted with another moleculre of the adduct, regenerating Fe(III)TPEN. In the cyt. c method with catalase, this Fe(III)TPEN-superoxide complex showed cyt.c oxidation activity , which had led to overstimation of its SOD activity. Based on the titration data, the main species of complex in aqueous media at neutral pH was indicated to be Fe(III)TPEN(OH^-). A spectral chagne after the reduction with hydrated electron indicates that the OH^- ion coordinates directly to Fe(III) by displacing one of the pyridine rings. The X-ray analysis of [Fe(II)TPEN]SO_4 supported this structure. From the above results we propose a novel reaction mechanism of FeTPEN and superoxide which resembles a proton catalyzed dismuting process, involving Fe(III)TPEN-superoxide complex.

• 社団法人日本薬学会の論文
• 2000-02-01

著者

• NAGANO Tetsuo

  Graduate School of Pharmaceutical Sciences, University of Tokyo

• Hirano Tomohisa

  Graduate School Of Pharmaceutical Sciences The University Of Tokyo

• Hirano Toshihiko

  Tokyo Univ. Medical Univ. Pharmacy And Life Sci. Tokyo Jpn

• Hirano Toshihiko

  Department Of Clinical Pharmacology Tokyo University Of Pharmacy And Life Science

• YAMAUCHI Osamu

  Department of Chemistry, Graduate School of Science, Nagoya University

• Yamauchi Osamu

  Department Of Chemistry Faculty Of Science Nagoya University

• Yamauchi Osamu

  Department Of Chemistry Faculty Of Sciences Nagoya Unicversity

• HIROBE Masaaki

  Graduate School of Pharmaceutical Sciences, The University of Tokyo

• KOBAYASHI Kazuo

  Institute of Scientific and Industrial Research, Osaka University

• ODANI Akira

  Department of Chemistry, Faculty of Sciences, Nagoya University

• OHSAWA Masanori

  Graduate School of Pharmaceutical Sciences, The University of Tokyo

• SATOW Yoshinori

  Graduate School of Pharmaceutical Sciences, The University of Tokyo

• Hirobe M

  Graduate School Of Pharmaceutical Sciences The University Of Tokyo

• Nagano T

  Lab. Of Chemistry And Biology Graduate School Of Pharmaceutical Sciences The Univ. Of Tokyo

• Nagano Tetsuo

  Graduate School Of Pharmaceutical Sciences The University Of Tokyo

• Odani Akira

  Department Of Chemistry Faculty Of Science Nagoya University

• Odani Akira

  Department Of Chemistry Faculty Of Sciences Nagoya University

• Hirano T

  Department Of Clinical Pharmacology Tokyo University Of Pharmacy And Life Science

• Ohsawa M

  Graduate School Of Pharmaceutical Sciences The University Of Tokyo

• Satow Yoshinori

  Graduate School Of Pharmaceutical Sciences The University Of Tokyo

• Kobayashi Kazuo

  Institute Of Scientific And Industrial Research Osaka University

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