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首页> 外文学位 >Organometallic photonucleases. I. DNA cleavage by the photolysis of cyclopentadienyl metal complexes: Mechanistic studies and sequence selectivity of strand scission by CpW(CO)3CH3. II. Footprinting of chromatin structure and chromatin remodeling by SWI/SNF utilizing CpW(CO)3CH3. III. Dual mechanisms of DNA damage by MoX(eta3-allyl)(CO)3(phen) complexes.
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Organometallic photonucleases. I. DNA cleavage by the photolysis of cyclopentadienyl metal complexes: Mechanistic studies and sequence selectivity of strand scission by CpW(CO)3CH3. II. Footprinting of chromatin structure and chromatin remodeling by SWI/SNF utilizing CpW(CO)3CH3. III. Dual mechanisms of DNA damage by MoX(eta3-allyl)(CO)3(phen) complexes.

机译：有机金属光核酸酶。 I.通过环戊二烯基金属配合物的光解来切割DNA：通过CpW（CO）3CH3进行断裂的机理研究和序列选择性。二。 SWI / SNF利用CpW（CO）3CH3进行染色质结构足迹测定和染色质重塑。三， MoX（eta3-烯丙基）（CO）3（phen）复合物对DNA的双重破坏机制。

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摘要

The photolysis of CpW(CO)3CH3 has been shown to produce methyl radicals and to cleave DNA in a single-stranded manner, and preliminary evidence implicated a carbon-centered radical in this process. In this work, the mechanism of strand scission in this reaction was determined to occur by hydrogen atom abstraction from the 4'- and 5'-positions of the deoxyribose moiety of the backbone of DNA. Additionally, in a side reaction that does not lead to frank strand scission, all four bases of DNA are methylated under these conditions; however, none of these base or backbone modifications lead to the formation of abasic sites.;Given the ideal characteristics of CpW(CO)3CH3 as a footprinting agent, it was utilized in footprinting studies to determine the higher order packing of nucleosomes in chromatin as well as to determine the structural changes that occur during chromatin remodeling by the SWI/SNF complex. While this reagent shows promise as a footprinting agent, more studies are needed to fine-tune the footprinting reaction.;In addition, dual mechanisms of DNA damage are reported for MoX(eta 3-allyl)(CO)2(phen) complexes, where X = H or X = CH 3. These complexes have been shown to cleave DNA in a single-stranded fashion non-sequence specific fashion via hydrogen atom abstraction from the H1' and/or the H5' of the deoxyribose moiety. In addition a G-selective DNA cleavage mechanism is observed under non-irradiated conditions. The products of this cleavage have been observe to be methylguanine, 8-methoxyguanine, and 8-oxo-guanine, as determined by mass spectral analysis.
机译：CpW（CO）3CH3的光解已显示会产生甲基自由基并以单链方式切割DNA，并且初步证据表明该过程涉及以碳为中心的自由基。在这项工作中，该反应中链断裂的机理是通过从DNA骨架的脱氧核糖部分的4'和5'位置提取氢原子而确定的。另外，在不会导致直链断裂的副反应中，在这些条件下，所有四个碱基的DNA都被甲基化。然而，这些碱基或骨架的修饰均未导致无碱基位点的形成。鉴于CpW（CO）3CH3作为足迹剂的理想特性，它被用于足迹研究中以确定染色质中核小体的高阶堆积。以及确定SWI / SNF复合物在染色质重塑过程中发生的结构变化。虽然该试剂显示出作为足迹剂的前景，但仍需要进行更多的研究以微调足迹反应。此外，据报道，MoX（η3-烯丙基）（CO）2（phen）配合物具有DNA损伤的双重机制，其中X ＝ H或X ＝ CH 3。这些复合物已显示通过从脱氧核糖部分的H1'和/或H5'夺氢原子以单链非序列特异性方式切割DNA。另外，在非辐照条件下观察到G-选择性DNA切割机制。如通过质谱分析所确定的，已经观察到该裂解的产物是甲基鸟嘌呤，8-甲氧基鸟嘌呤和8-氧代鸟嘌呤。

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  • 作者

    Downs, Jennifer.;

  • 作者单位

    Emory University.;

  • 授予单位 Emory University.;
  • 学科 Chemistry Organic.
  • 学位 Ph.D.
  • 年度 2005
  • 页码 142 p.
  • 总页数 142
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
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