Chromium(IV)-Peroxo Complex Formation and Its Nitric Oxide Dioxygenase Reactivity

被引：60

作者：

Yokoyama, Atsutoshi ^{[1
]}

Han, Jung Eun ^{[1
]}

Cho, Jaeheung ^{[1
]}

Kubo, Minoru ^{[2
]}

Ogura, Takashi ^{[2
]}

Siegler, Maxime A. ^{[3
]}

Karlin, Kenneth D. ^{[1
,3
]}

Nam, Wonwoo ^{[1
]}

机构：

[1] Ewha Womans Univ, Dept Bioinspired Sci, Seoul 120750, South Korea

[2] Univ Hyogo, Grad Sch Life Sci, Picobiol Inst, Hyogo, Japan

[3] Johns Hopkins Univ, Dept Chem, Baltimore, MD 21218 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2012年 / 134卷 / 37期

基金：

美国国家卫生研究院;

关键词：

ELECTRON-PARAMAGNETIC-RESONANCE; SPECTROSCOPIC CHARACTERIZATION; COORDINATION CHEMISTRY; ACTIVATION; BEARING; MODELS;

D O I：

10.1021/ja307384e

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The O-2 and NO reactivity of a Cr(II) complex bearing a 12-membered tetraazamacrocyclic N-tetramethylated cyclam (TMC) ligand, [Cr-II(12-TMC)-(Cl)](+) (1), and the NO reactivity of its peroxo derivative, [Cr-IV(12-TMC)(O-2)(Cl)](+) (2), are described. By contrast to the previously reported Cr(III)-superoxo complex, [Cr-III(14-TMC)(O-2)(Cl)](+), the Cr(IV)-peroxo complex 2 is formed in the reaction of 1 and O-2. Full spectroscopic and X-ray analysis revealed that 2 possesses side-on eta(2)-peroxo ligation. The quantitative reaction of 2 with NO affords a reduction in Cr oxidation state, producing a Cr(III)-nitrato complex, [Cr-III(12-TMC)(NO3)(Cl)](+) (3). The latter is suggested to form via a Cr(III)- peroxynitrite intermediate. [Cr-II(12-TMC)(NO)(Cl)](+) (4), a Cr(II)-nitrosyl complex derived from 1 and NO, could also be synthesized; however, it does not react with O-2.

引用

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页码：15269 / 15272

页数：4

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