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Nucleic Acids Research Advance Access published online on May 8, 2008
Nucleic Acids Research, doi:10.1093/nar/gkn244
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© 2008 The Author(s)
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-nc/2.0/uk/) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.

Chemistry

DNA binding of dinuclear iron(II) metallosupramolecular cylinders. DNA unwinding and sequence preference

Jaroslav Malina1, Michael J. Hannon2 and Viktor Brabec1,*

1Institute of Biophysics, Academy of Sciences of the Czech Republic, v.v.i., Královopolská 135, CZ-61265 Brno, Czech Republic and 2School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT, UK

*To whom correspondence should be addressed. Tel: +420 541517148; Fax: +420 51412499; Email: brabec{at}ibp.cz

Received March 1, 2008. Revised April 5, 2008. Accepted April 16, 2008.

[Fe2L3]4+ (L = C25H20N4) is a synthetic tetracationic supramolecular cylinder (with a triple helical architecture) that targets the major groove of DNA and can bind to DNA Y-shaped junctions. To explore the DNA-binding mode of [Fe2L3]4+, we examine herein the interactions of pure enantiomers of this cylinder with DNA by biochemical and molecular biology methods. The results have revealed that, in addition to the previously reported bending of DNA, the enantiomers extensively unwind DNA, with the M enantiomer being the more efficient at unwinding, and exhibit preferential binding to regular alternating purine–pyrimidine sequences, with the M enantiomer showing a greater preference. Also, interestingly, the DNA binding of bulky cylinders [Fe2(L-CF3)3]4+ and [Fe2(L-Ph)3]4+ results in no DNA unwinding and also no sequence preference of their DNA binding was observed. The observation of sequence-preference in the binding of these supramolecular cylinders suggests that a concept based on the use of metallosupramolecular cylinders might result in molecular designs that recognize the genetic code in a sequence-dependent manner with a potential ability to affect the processing of the genetic code.


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