Hydrogen peroxide and dioxygen activation by dinuclear copper complexes in aqueous solution: Hydroxyl radical production initiated by internal electron transfer

被引：0

作者：

Zhu, Qing ^{[1
]}

Lian, Yuxiang ^{[2
]}

Thyagarajan, Sunita ^{[2
]}

Rokita, Steven E. ^{[1
]}

Karlin, Kenneth D. ^{[2
]}

Blough, Neil V. ^{[1
]}

机构：

[1] Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, United States

[2] Department of Chemistry, Johns Hopkins University, Baltimore, MD 21218, United States

来源：

Journal of the American Chemical Society | 2008年 / 130卷 / 20期

关键词：

Dinuclear Cu(II) complexes; CuII2Nn; (n; 4; or; 5); were recently found to specifically cleave DNA in the presence of a reducing thiol and O2 or in the presence of H2O2 alone. However; CuII2N3 and a closely related mononuclear Cu(II) complex exhibited no selective reaction under either condition. Spectroscopic studies indicate an intermediate is generated from CuII2Nn (n = 4 or 5) and mononuclear Cu(II) solutions in the presence of H2O2 or from CuI2Nn (n = 4 or 5) in the presence of O2. This intermediate decays to generate OH radicals and ligand degradation products at room temperature. The lack of reactivity of the intermediate with a series of added electron donors suggests the intermediate discharges through a rate-limiting intramolecular electron transfer from the ligand to the metal peroxo center to produce an OH radical and a ligand-based radical. These results imply that DNA cleavage does not result from direct reaction with a metal-peroxo intermediate but instead arises from reaction with either OH radicals or ligand-based radicals. Copyright © 2008 American Chemical Society;

D O I：

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学科分类号：

摘要：

Journal article (JA)

引用

页码：6304 / 6305

共 35 条

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Zhu, Qing
Lian, Yuxiang
Thyagarajan, Sunita
Rokita, Steven E.
Karlin, Kenneth D.
Blough, Neil V.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (20) : 6304 - +
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ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2015, 49 (17) : 10373 - 10379
[4] RADICAL INITIATED SYNTHESIS OF HYDROXYL TERMINATED POLYMERS USING AQUEOUS HYDROGEN-PEROXIDE AS INITIATOR
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CHEMICAL & PHARMACEUTICAL BULLETIN, 1992, 40 (05) : 1087 - 1089
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Wang, Haocun
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Bian, Junjie
Li, Chunhu
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2024, 12 (06):
[8] MEASUREMENT OF ACTIVATION-ENERGY FOR REACTION OF HYDROXYL RADICAL WITH HYDROGEN IN AQUEOUS-SOLUTION
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ADVANCES IN INORGANIC CHEMISTRY: INCLUDING BIOINORGANIC STUDIES, VOL 55, 2004, 55 : 1 - 59
[10] COPPER, ZINC SUPEROXIDE-DISMUTASE CATALYZES HYDROXYL RADICAL PRODUCTION FROM HYDROGEN-PEROXIDE
YIM, MB
CHOCK, PB
STADTMAN, ER
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1990, 87 (13) : 5006 - 5010

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