期刊
BIOCHEMISTRY
卷 50, 期 19, 页码 4155-4161出版社
AMER CHEMICAL SOC
DOI: 10.1021/bi200201n
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资金
- Slovenian research agency (ARRS)
- Ministry of higher education, science and technology of the Republic of Slovenia [P1-0242, J1-0986]
- EU [228461, 261863]
G-Rich oligonucleotides with cytosine residues in their sequences can form G-quadruplexes where G-quartets are flanked by G.C Watson-Crick base pairs. In an attempt to probe the role of cations in stabilization of a structural element with two G.C base pairs stacked on a G-quartet, we utilized solution state nuclear magnetic resonance to study the folding of the d(G(3)CT(4)G(3)C) oligonucleotide into a G-quadruplex upon addition of (NH4+)-N-15 ions. Its bimolecular structure exhibits antiparallel strands with edge-type loops. Two G-quartets in the core of the structure are flanked by a couple of Watson Crick G.C base pairs in a sheared arrangement. The topology is equivalent to the solution state structure of the same oligonucleotide in the presence of Na+ and K+ ions [Kettani, A., et al. (1998) J. Mol. Biol. 282, 619, and Bouaziz, S., et al. (1998) J. MoL Biol. 282, 637). A single ammonium ion binding site was identified between adjacent G-quartets, but three sites were expected. The remaining potential cation binding sites between G-quartets and G.C base pairs are occupied by water molecules. This is the first observation of long-lived water molecules within a G-quadruplex structure. The flanking G C base pairs adopt a coplanar arrangement and apparently do not require cations to neutralize unfavorable electrostatic interactions among proximal carbonyl groups. A relatively fast movement of ammonium ions from the inner binding site to bulk with the rate constants of 21 s(-1) was attributed to the lack of hydrogen bonds between adjacent G.C base pairs and the flexibility of the T-4 loops.
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