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首页> 外文期刊>Chemistry: A European journal >Competitive Reactions of Interstrand and Intrastrand DNA-Pt Adducts: A Dinuclear-Platinum Complex Preferentially Forms a 1,4-Interstrand Cross-Link Rather than a 1,2 Intrastrand Cross-link on Binding to a GG 14-Mer Duplex
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Competitive Reactions of Interstrand and Intrastrand DNA-Pt Adducts: A Dinuclear-Platinum Complex Preferentially Forms a 1,4-Interstrand Cross-Link Rather than a 1,2 Intrastrand Cross-link on Binding to a GG 14-Mer Duplex

机译：链间和链内DNA-Pt加合物的竞争反应：双核-铂络合物优先形成1,4-链间交联而不是与GG 14-Mer双链体结合时形成1,2链内交联。

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摘要

A study of the kinetics and mechanism of the reaction between the dinuclear Pt complex [{trans-PtCl(NH_3)_2}_2(mu-NH_2(CH_2)_6NH_2)]~(2+) (1) and the 14-mer duplex 5'-d(ATACATG(7)G(8)TACATA)-3'·5'-d(TATG(25)TACCATG(18)TAT)-3' is reported. [~1H, ~15N]-HSQC NMR was used to follow the reaction at 298 K, pH 5.4. The production cross-link between G(8) and G(18) bases and exists in two conformational forms. No evidence for the possible 1,2-intrastrand G(7)G(8) adduct was seen, confirming the preferential formation of interstrand cross-links by these dinuclear complexes. An initial electrostatic association of ~15N-1 with the duplex is indicated by changes in its ~1H/~15N chemical shifts, followed by aquation of 1 to form the monoaqua monochloro species 2, with a rate constant of 4.00 (+-) 0.03 X10~(-5) s~(-1). Monofunctional binding to the duplex occurs primarily at G(8), the 3' base of the nucleophilic GG grouping, with a rate constant of 1.5 (+-) 0.7 M~(-1) s~(-1). Changes in the ~1H/~15N shifts indicate there is an electrostatic interaction between the unbound {PtN_3Cl} group of the monofunctional adduct and the duplex. No peaks for a transient aquated monofunctional species are seen and closure of 3 to form the 1,4-G(8)G(18) interstrand cross-link (5) was treated as direct, with a rate constant of 4.47 (+-) 0.06 X 10~(-5) s~(-1). The G(8)G(18) cross-link was confirmed from analysis of the NOESY NMR spectrum of the final product. Structural perturbations for the 1,4-interstrand cross-link extend over approximately four base-pairs and are similar to those found for a 1,4-interstrand cross-link with a shorter 8-mer -GTAC-sequence. A major distortion was evident for the 5T (T(17)) adjacent to the platinated G(18), consistent with the findings from the use of chemical probes to investigate the conformation of 1,4-interstrand cross-links.
机译：双核铂络合物[{trans-PtCl（NH_3）_2} _2（mu-NH_2（CH_2）_6NH_2）]〜（2+）（1）与14-mer双链体反应的动力学和机理研究据报道5'-d（ATACATG（7）G（8）TACATA）-3'·5'-d（TATG（25）TACCATG（18）TAT）-3'。 [〜1H，〜15N] -HSQC NMR用于在298 K，pH 5.4下跟踪反应。 G（8）和G（18）碱基之间的生产交联，并以两种构象形式存在。没有证据表明可能的1,2-链内G（7）G（8）加合物，证实这些双核复合物优先形成链间交联。 〜15N-1与双链体之间的初始静电缔合由其〜1H /〜15N化学位移的变化指示，然后由1水化形成单水一氯物种2，速率常数为4.00（+-）0.03 X10〜（-5）s〜（-1）。与双链体的单官能结合主要发生在亲核GG分组的3'碱基G（8）处，速率常数为1.5（±）0.7 M〜（-1）s〜（-1）。 〜1H /〜15N位移的变化表示单官能加合物的未结合{PtN_3Cl}基团与双链体之间存在静电相互作用。没有看到短暂的水合单功能物质的峰，将3形成1，4-G（8）G（18）链间交联（5）的闭合视为直接峰，速率常数为4.47（+- ）0.06 X 10〜（-5）s〜（-1）。 G（8）G（18）交联是由最终产品的NOESY NMR光谱分析确定的。 1,4-链间交联的结构扰动在大约四个碱基对上延伸，类似于具有较短的8-mer-GTAC序列的1,4-链间交联的结构扰动。 5T（T（17））靠近镀铂G（18）的主要畸变是明显的，这与使用化学探针研究1,4-链间交联构象的发现是一致的。

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