Impact of metal coordination on cytotoxicity of 3-aminopyridine-2- carboxaldehyde thiosemicarbazone (Triapine) and novel insights into terminal dimethylation

Author(s)
Christian Kowol, Robert Trondl, Petra Heffeter, Vladimir Arion, Michael Jakupec, Alexander Roller, Mathea Sophia Galanski, Walter Berger, Bernhard Keppler
Abstract

The first metal complexes of 3-aminopyridine-2-carboxaldehyde thiosemicarbazone (Triapine) were synthesized. Triapine was prepared by a novel three-step procedure in 64% overall yield. In addition, a series of related ligands, namely, 2-formylpyridine thiosemicarbazone, 2-acetylpyridine thiosemicarbazone, 2-pyridineformamide thiosemicarbazone, and their N 4-dimethylated derivatives (including the N4-dimethylated analogue of Triapine) were prepared, along with their corresponding gallium(III) and iron(III) complexes with the general formula [M(L)2] +, where HL is the respective thiosemicarbazone. The compounds were characterized by elemental analysis, 1H and 13C NMR, IR and UV-vis spectroscopies, mass spectrometry, and cyclic voltammetry. In addition, Triapine and its iron(III) and gallium(III) complexes were studied by X-ray crystallography. All ligands and complexes were tested for their in vitro antiproliferative activity in two human cancer cell lines (41M and SK-BR-3), and structure-activity relationships were established. In general, the coordination to gallium(III) increased the cytotoxicity while the iron(III) complexes show reduced cytotoxic activity compared to the metal-free thiosemicarbazones. Selected compounds were investigated for the capacity of inhibiting ribonucleotide reductase by incorporation of 3H-cytidine into DNA.

Organisation(s)
Department of Inorganic Chemistry
External organisation(s)
Medizinische Universität Wien
Journal
Journal of Medicinal Chemistry
Volume
52
Pages
5032-5043
No. of pages
12
ISSN
0022-2623
DOI
https://doi.org/10.1021/jm900528d
Publication date
2009
Peer reviewed
Yes
Austrian Fields of Science 2012
104003 Inorganic chemistry, 104002 Analytical chemistry, 301114 Cell biology
Sustainable Development Goals
SDG 3 - Good Health and Well-being
Portal url
https://ucrisportal.univie.ac.at/en/publications/2f5ac294-d3f4-44d0-b842-a2bc2f0c32ac