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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Exchangeable proton ENDOR as a probe of the redox-active iron center in activated bleomycin and ferric bleomycin
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Exchangeable proton ENDOR as a probe of the redox-active iron center in activated bleomycin and ferric bleomycin

机译：可更换的质子末端作为活化的博来霉素和博莱霉素的氧化还原活性铁中心的探针

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Activated bleomycin (ABLM) is a drug-Fe(III)-hydroperoxide complex kinetically competent in DNA attack (via H4 ' abstraction). This intermediate is relatively stable, but its spontaneous conversion to ferric bleomycin (Fe(III).BLM) is poorly characterized because no observable intermediate product accumulates. The Fe(III).BLM formed cryophotolytically from ABLM and kept at 77 K was remarkably similar by EPR and ENDOR criteria to Fe(III).BLM formed from Fe(III) + BLM solution. The notable ENDOR criteria were the ENDOR frequencies and features of orientation-selected, strongly hyperfine-coupled, exchangeable protons associated with the environs of the iron within < 3.5 angstrom of paramagnetic Fe(III) in Fe(III).BLM and ABLM. Cryophotolytic conversion of activated bleomycin to its ferric bleomycin product in the frozen solid is a sign that the reaction requires only constrained local proton rearrangements. We have characterized the metal-proton distances and orientations of the protons in that rearrangement, especially noting that these protons are of mechanistic importance in the ambient temperature conversion of ABLM to Fe(III).BLM in concert with a directed radical-forming attack on DNA.
机译：活化的Bleomycin（ABLM）是DNA攻击中的药物 - Fe（III） - 氢氧化氢络合物（通过H4'抽象）。该中间体相对稳定，但其自发转化为FERROMYCIN（Fe（III）.BLM）的特征差异很差，因为没有可观察到的中间产物积累。通过EPR和ENDOR标准与ABLM的低温和77K保持在77k的FE（III）.BLM与FE（III）.BLM由Fe（III）+ BLM溶液形成非常相似。值得注意的内或标准是与铁在Fe（III）中的顺磁FE（III）的3.5埃·埃克斯特射线中的铁环偶联，与铁的环境相关联的内频和耦合，可交换的质子的结合频率和特征.BLM和ABLM。在冷冻固体中激活的玻璃霉素在其透气霉素产物中转化的低温解力转化是反应仅需要受约束的局部质子重排的标志。我们已经表征了该重排中的金属质子距离和质子的取向，特别是注意这些质子在ABLM到Fe（III）的环境温度转换中的机械重视.BLM与一定的激进形成攻击脱氧核糖核酸。

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