博来霉素“活性复合物”的结构研究：在亚铁-博来霉素-一氧化碳复合物中配体与亚铁离子的分配
Structural studies of of "active complex" of bleomycin: assignment of ligands to the ferrous ion in a ferrous-bleomycin-carbon monoxide complex.
作者信息
Oppenheimer N J, Rodriguez L O, Hecht S M
出版信息
Proc Natl Acad Sci U S A. 1979 Nov;76(11):5616-20. doi: 10.1073/pnas.76.11.5616.
Abstract
Proton NMR studies at 360 MHz establish the binary Fe(II)-bleomycin complex to be paramagnetic with a spectrum covering 70 ppm. Addition of carbon monoxide generates a stable, diamagnetic Fe(II)-bleomycin-CO complex that is a putative structural analog of the "active" Fe(II)-bleomycin-O2 complex. The following six groups have been determined to be coordinated to the Fe(II) ion from analysis of the highly resolved 1H NMR spectra of this complex: CO, the primary and secondary amine nitrogens of the beta-aminoalanine moiety, the carbamoyl moiety on the 3-position of mannose, the pyrimidine N-1, and the imidazole N-1. The Fe(II)-bleomycin-CO complex binds to DNA, as shown by fluorescence quenching experiments, but Fe(II)-bleomycin-CO does not mediate thymine release. These results necessitate a major revision in the current model for metal coordination to bleomycin.
摘要
在360兆赫下进行的质子核磁共振研究表明，二元铁（II）-博来霉素络合物具有顺磁性，其光谱覆盖范围达70 ppm。一氧化碳的加入会生成一种稳定的抗磁性铁（II）-博来霉素-CO络合物，它被认为是“活性”铁（II）-博来霉素-O₂络合物的结构类似物。通过对该络合物高分辨率¹H核磁共振光谱的分析，已确定以下六个基团与铁（II）离子配位：CO、β-丙氨酸部分的伯胺和仲胺氮原子、甘露糖3位上的氨基甲酰部分、嘧啶N-1以及咪唑N-1。荧光猝灭实验表明，铁（II）-博来霉素-CO络合物能与DNA结合，但铁（II）-博来霉素-CO并不介导胸腺嘧啶的释放。这些结果使得目前关于金属与博来霉素配位的模型需要进行重大修订。
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