Structure of the complex of [Ru(tpm)(dppz)py](2+) with a B-DNA oligonucleotide - a single-substituent binding switch for a metallo-intercalator

Chemistry : a European Journal
Philip WaywellJames A Thomas

Abstract

We report the synthesis of three new complexes related to the achiral [Ru(tpm)(dppz)py](2+) cation (tpm=tripyridazole methane, dppz=dipyrido[3,2-a:2',3'-c]phenazine, py=pyridine) that contain an additional single functional group on the monodentate ancillary pyridyl ligand. Computational calculations indicate that the coordinated pyridyl rings are in a fixed orientation parallel to the dppz axis, and that the electrostatic properties of the complexes are very similar. DNA binding studies on the new complexes reveal that the nature and positioning of the functional group has a profound effect on the binding mode and affinity of these complexes. To explore the molecular and structural basis of these effects, circular dichroism and NMR studies on [Ru(tpm)(dppz)py]Cl(2) with the octanucleotides d(AGAGCTCT)(2) and d(CGAGCTCG)(2), were carried out. These studies demonstrate that the dppz ligand intercalates into the G(2)-A(3) step, with {Ru(tpm)py} in the minor groove. They also reveal that the complex intercalates into the binding site in two possible orientations with the pyridyl ligand of the major conformer making close contact with terminal base pairs. We conclude that substitution at the 2- or 3-position of the pyridine ring ha...Continue Reading

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Citations

Apr 22, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Michael G WalkerJim A Thomas
Jul 19, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Guanying LiHui Chao
Oct 20, 2012·Angewandte Chemie·Michael G WalkerJim A Thomas
Jun 24, 2010·ChemMedChem·Ruth BiedaWilliam S Sheldrick
Jun 19, 2013·Philosophical Transactions. Series A, Mathematical, Physical, and Engineering Sciences·James P HallChristine J Cardin
Jan 23, 2020·Chemical Communications : Chem Comm·Hiwa K SaeedJim A Thomas
Jan 29, 2013·Dalton Transactions : an International Journal of Inorganic Chemistry·Andrew W McKinleyEimer M Tuite
Oct 8, 2013·Acta Crystallographica. Section E, Structure Reports Online·Benjamin J CoeDaniela Rusanova
Oct 15, 2014·Journal of Medicinal Chemistry·Huaiyi HuangHui Chao

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