NMR studies of the paramagnetic complex Fe(II)-bleomycin

被引:65
|
作者
Lehmann, TE
Ming, LJ
Rosen, ME
Que, L
机构
[1] UNIV MINNESOTA,DEPT CHEM,MINNEAPOLIS,MN 55455
[2] UNIV MINNESOTA,CTR MET BIOCATALYSIS,MINNEAPOLIS,MN 55455
[3] UNIV S FLORIDA,DEPT CHEM,TAMPA,FL 33620
[4] UNIV S FLORIDA,INST BIOMOL SCI,TAMPA,FL 33620
关键词
D O I
10.1021/bi962748t
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
The coordination chemistry of the iron(II) complex of the antitumor drug bleomycin has been extensively investigated with a number of spectroscopic and chemical techniques. However, the actual structure of this complex is not established. in this report, we present NMR studies of the paramagnetic Fe(II)BLM and use one- and two-dimensional methods to assign the paramagnetically shifted features to particular protons. The data analysis points toward the primary and secondary amines of the beta-aminoalanine fragment, the pyrimidine and imidazole rings, and the amide nitrogen of the beta-hydroxyhistidine fragment as ligands to the metal center. Correlation of the T-1 values with the metal-proton distances derived from the NMR-generated solution structure of HOO-Co(III)BLM [Wu, W., Vanderwall, D. E., Lui, S. M., Tang, X.-J., Turner, C. J., Kozarich, J. W., & Stubbe, J. (1996) J. Am. Chem. Sec. 118, 1268-1280] indicates that the two metallobleomycins share similar structures. The chemical shifts as well as the T-1 values of the sugar protons indicate that these fragments are close but not bound to the metal in Fe(II)BLM.
引用
收藏
页码:2807 / 2816
页数:10
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