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Isotopic Labeling Experiments That Elucidate the Mechanism of DNA Strand Cleavage by the Hypoxia-Selective Antitumor Agent 1,2,4-Benzotriazine 1,4-Di-N-oxide
Chemical Research in Toxicology
  • Xiulong Shen
  • Anuruddha Rajapakse
  • Fabio A. Gallazzi
  • Venkatraman Junnotula
  • Tarra Fuchs-Knotts
  • Rainer Glaser, Missouri University of Science and Technology
  • Kent S. Gates
Abstract

The 1,2,4-benzotriazine 1,4-dioxides are an important class of potential anticancer drugs that selectively kill the low-oxygen (hypoxic) cells found in solid tumors. These compounds undergo intracellular one-electron enzymatic reduction to yield an oxygen-sensitive drug radical intermediate that partitions forward, under hypoxic conditions, to generate a highly reactive secondary radical that causes cell killing DNA damage. Here, we characterized bioreductively activated, hypoxia-selective DNA-strand cleavage by 1,2,4-benzotriazine 1,4-dioxide. We found that one-electron enzymatic activation of 1,2,4-benzotriazine 1,4-dioxide under hypoxic conditions in the presence of the deuterium atom donor methanol-d4 produced nondeuterated mono-N-oxide metabolites. This and the results of other isotopic labeling studies provided evidence against the generation of atom-abstracting drug radical intermediates and are consistent with a DNA-damage mechanism involving the release of hydroxyl radical from enzymatically activated 1,2,4-benzotriazine 1,4-dioxides.

Department(s)
Chemistry
Keywords and Phrases
  • 1,2,4 benzotriazine 1,4 dioxide,
  • deuterium,
  • hydroxyl radical,
  • methanol,
  • 1,2,4-benzotriazine 1,4-di-N-oxide,
  • amine oxide,
  • antineoplastic agent,
  • triazine derivative,
  • controlled study,
  • cytotoxicity,
  • DNA cleavage,
  • DNA damage,
  • DNA strand,
  • enzyme activation,
  • isotope labeling,
  • anoxia,
  • chemical structure,
  • chemistry,
  • DNA cleavage,
  • drug effects,
  • metabolism,
  • Anoxia,
  • Antineoplastic Agents,
  • Cyclic N-Oxides,
  • DNA Cleavage,
  • Isotope Labeling,
  • Molecular Structure,
  • Triazines
Document Type
Article - Journal
Document Version
Citation
File Type
text
Language(s)
English
Rights
© 2014 American Chemical Society (ACS), All rights reserved.
Publication Date
12-1-2014
Publication Date
01 Dec 2014
Disciplines
Citation Information
Xiulong Shen, Anuruddha Rajapakse, Fabio A. Gallazzi, Venkatraman Junnotula, et al.. "Isotopic Labeling Experiments That Elucidate the Mechanism of DNA Strand Cleavage by the Hypoxia-Selective Antitumor Agent 1,2,4-Benzotriazine 1,4-Di-N-oxide" Chemical Research in Toxicology Vol. 27 Iss. 1 (2014) p. 111 - 118 ISSN: 0893-228X; 1520-5010
Available at: http://works.bepress.com/rainer-glaser/113/