Catalytic Reduction of O_2 by Pyrazine Derivatives

Rong Wang; Takeyoshi Okajima; Fusao KitamuraSusumu KawauchiNaoki MatsumotoThies ThiemannShuntaro MatakaTakeo Ohsaka

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Catalytic Reduction of O_2 by Pyrazine Derivatives

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The catalytic reduction of molecular oxygen (O_2) by four kinds of pyrazine derivatives-2,3,5,6-tetramethylpyrazine, 2,3-dimethylquinoxaline, 2,3-diphenylquinoxaline, and phenazine-has been studied by cyclic and rotating disk voltammetry and molecular orbital calculations using the MOPAC PM5 method. In sufficiently acidic solution (pH ≈ 1), the pyrazine derivatives underwent two successive one-electron reductions. Therefore, it was possible to compare the reactivity of both one-electron reduced forms (the radicals) and two-electron reduced forms of the derivatives toward O_2 in this acidic solution. Theoretical calculations showed that all of the redox forms of the derivatives are protonated to be cations in this solution and that all of the reduced forms, except for that of phenazine, react with O_2. The rate constants (k_1) of the second-order reactions of the reduced forms with O_2 were estimated by rotating disk voltammetry. A linear relationship between log(k_1) and the half-wave potential (E1/2) of the one-electron and two-electron reduced forms was observed, indicating that the catalytic reduction of O_2 proceeds by a common reaction mechanism and that its rate constant depends on its thermodynamic driving force.

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2004年第11期|1891-1899|共9页
作者
Rong Wang; Takeyoshi Okajima; Fusao KitamuraSusumu KawauchiNaoki MatsumotoThies ThiemannShuntaro MatakaTakeo Ohsaka;
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作者单位

Department of Electronic Chemistry, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8502, Japan;

Department of Organic and Polymeric Materials, Graduate School of Science and Engineering, Tokyo Institute of Technology, O-okayama 2-12-1, Meguro-ku, Tokyo 152-8552, Japan;

Institute for Materials Chemistry and Engineering, Kyushu University, 6-1 Kasuga-koh-en, Kasuga-shi, Fukuoka 816-8580, Japan;

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正文语种英语
中图分类物理化学（理论化学）、化学物理学;
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Catalytic Reduction of O_2 by Pyrazine Derivatives

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