Solution Structure of Fe(II)-azide-bleomycin Derived from NMR Data: Transition from Fe(II)-bleomycin to Fe(II)-azide-bleomycin As Derived from NMR Data and Structural Calculations

Overview

Journal J Biol Inorg Chem

Publisher Springer

Specialty Biochemistry

Date 2012 Apr 7

PMID 22481631

Citations 4

Authors

Teresa Lehmann

Yang Li

Affiliations

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Abstract

The coordination cage of the metal center in Fe(II)-bleomycin has been proposed to consist of the secondary amines in β-aminoalanine, the pyrimidinylpropionamide and imidazole rings, and the amide nitrogen in β-hydroxyhistidine as equatorial ligands, and the primary amine in β-aminoalanine and either the carbamoyl group in mannose or a solvent molecule occupying the axial sites. With the aim of supporting or not supporting coordination of a water molecule to the metal center in Fe(II)-bleomycin, the solution structure of Fe(II)-azide-bleomycin has been derived from NMR data. The structural changes that occur in Fe(II)-bleomycin upon azide binding have been monitored by comparing the experimental results with those obtained from the calculated structures for both bleomycin adducts. The results of this investigation strongly support a model of Fe(II)-bleomycin with six endogenous ligands as the most likely structure held in solution by this metallobleomycin in the absence of DNA.

Citing Articles

Structural changes of Zn(II)bleomycin complexes when bound to DNA hairpins containing the 5'-GT-3' and 5'-GC-3' binding sites studied through NMR spectroscopy.

Follett S, Murray S, Ingersoll A, Reilly T, Lehmann T Magnetochemistry. 2018; 4(1).

PMID: 30464999 PMC: 6241535. DOI: 10.3390/magnetochemistry4010004.

Interaction of Zn(II)bleomycin-A and Zn(II)peplomycin with a DNA hairpin containing the 5'-GT-3' binding site in comparison with the 5'-GC-3' binding site studied by NMR spectroscopy.

Follett S, Ingersoll A, Murray S, Reilly T, Lehmann T J Biol Inorg Chem. 2017; 22(7):1039-1054.

PMID: 28748309 PMC: 5985968. DOI: 10.1007/s00775-017-1482-z.

NMR study of the effects of some bleomycin C-termini on the structure of a DNA hairpin with the 5'-GC-3' binding site.

Lehmann T, Murray S, Ingersoll A, Reilly T, Follett S, Macartney K J Biol Inorg Chem. 2016; 22(1):121-136.

PMID: 27858165 PMC: 5950717. DOI: 10.1007/s00775-016-1413-4.

Contributions of NMR to the understanding of the coordination chemistry and DNA interactions of metallo-bleomycins.

Lehmann T, Topchiy E Molecules. 2013; 18(8):9253-77.

PMID: 23917114 PMC: 6270211. DOI: 10.3390/molecules18089253.

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