期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 24, 期 58, 页码 15577-15588出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201802147
关键词
DNA recognition; G-quadruplexes; light switches; ruthenium complexes
资金
- Fonds de la Recherche Scientifique-FNRS (Belgium) [1.B333.15F, F.4532.16, 2.4530.12, 2.4615.11, UN02715F, CDR J.0022.18]
- Interuniversity Attraction Poles Programme [PAI 7/05]
- Belgian Science Policy Office
- Fonds pour la Formation a la Recherche dans l'Industrie et dans l'Agriculture (FRIA)
- Institut National de la Sante et de la Recherche Medicale (INSERM)
- Nouvelle Aquitaine Region
- Czech Science Foundation [P208/12/G016]
- National Program of Sustainability I from the Ministry-of-Youth, Education and Sports of the Czech Republic [LO1305]
Metal complexes constitute an important class of DNA binders. In particular, a few ruthenium polyazaaromatic complexes are attractive as light switches because of their strong luminescence enhancement upon DNA binding. In this paper, a comprehensive study on the binding modes of several mononuclear and binuclear ruthenium complexes to human telomeric sequences, made of repeats of the d(TTAGGG) fragment is reported. These DNA sequences form G-quadruplexes (G4s) at the ends of chromosomes and constitute a relevant biomolecular target in cancer research. By combining spectroscopy experiments and molecular modelling simulations, several key properties are deciphered: the binding modes, the stabilization of G4 upon binding, and the selectivity of these complexes towards G4 versus double-stranded DNA. These results are rationalized by assessing the possible deformation of G4 and the binding free energies of several binding modes via modelling approaches. Altogether, this comparative study provides fundamental insights into the molecular recognition properties and selectivity of Ru complexes towards this important class of DNA G4s.
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