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首页> 外文期刊>Chemistry: A European journal >Facile Preparation of Pt~II-Nucleobase Monoadducts iwth trans Geometry: Structural Characterization and kinetics for Cl~- Hydrolysis Reactions of trans-[PtCl(NH_3)_2(L-N7)]~n+ (L = 9-Methyladenine or 9-Methylhypoxanthine)
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Facile Preparation of Pt~II-Nucleobase Monoadducts iwth trans Geometry: Structural Characterization and kinetics for Cl~- Hydrolysis Reactions of trans-[PtCl(NH_3)_2(L-N7)]~n+ (L = 9-Methyladenine or 9-Methylhypoxanthine)

机译：反式几何结构简便地制备Pt〜II-核碱基一加合物：反式[[PtCl（NH_3）_2（L-N7）]〜n +（L = 9-甲基腺嘌呤或9-甲基次黄嘌呤）的Cl〜-水解反应的结构表征和动力学）

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摘要

The employment of trans[PtCl(OH)(NH_3)_2.H_2O as the platinum source offers a convenient and efficient way to prepare 1:1 adducts with the model nucleobases 9-methyladenine (9-MeAde) and 9-methylhypoxanthine (9-MeHypH). The resulting complexes, trans-[Pl(NH_3)_2(9-MeAde-N7)]ClO_4 and trans-[PtCl(NH_3)_2(9-MeHyp-N7)]. 2H_2O, were structurally characterized by X-ray crystalography. The crystal packing of both complexes is stabilized by a hydrogen-bonding network involving primarily NH_3 ligands and perchlorate oxygens in trans-[PtCl(NH_3)_2-(9-MeAde-N7)]ClO_4, adn NH_3 ligands and the C(6)O group of the nucleobase in trans-[PtCl(NH_3)_2(9-MeHyp-N7)]. 2H_2O. There hydrogne bonds to the oxo group in the latter compound suggest that the negative charge caused by N1H deprotonation of the nucleobase is partly located on the oxygen atom; this is supported by the slightly larger downfield shift of C(6) over C(2) in the ~13C spectrum. However, the anticipated lengthening of the C(6)-O(6) bond upon N1H deprotonation was not verified by X-ray results. Kinetics for the Clhydrolysis in basic aqueous solution were followed by ~195Pt NMR and HPLC analysis, which showed the formation of only one product in both cases with a ~195t hcemial shift typical for a PtN_3O coordination sphere. The comparable kinetic data found by these two methods reveal that the water molecule acts as the nucleophile in the hydrolysis reactions and that it displaces the Cl~- ligand more readily in the 9-methyladenine complex.
机译：使用trans [PtCl（OH）（NH_3）_2.H_2O作为铂源提供了一种方便有效的方法，可使用模型核碱基9-甲基腺嘌呤（9-MeAde）和9-甲基次黄嘌呤（9- MeHypH）。所得的复合物，反式-[Pl（NH_3）_2（9-MeAde-N7）] ClO_4和反式-[PtCl（NH_3）_2（9-MeHyp-N7）]。 X射线晶体学表征2 H_2O。两种配合物的晶体堆积均通过氢键网络稳定化，该网络主要包含NH_3配体和高氯酸盐中的反式-[PtCl（NH_3）_2-（9-MeAde-N7）] ClO_4，adn NH_3配体和C（6）反式-[PtCl（NH_3）_2（9-MeHyp-N7）]中核碱基的O组。 2H_2O。后一种化合物中的氧代基上存在水合键，表明由核碱基的N1H去质子化引起的负电荷部分位于氧原子上。在〜13C频谱中，C（6）相对于C（2）的下场偏移略大，这证明了这一点。但是，X1射线结果未证实N1H去质子化时C（6）-O（6）键的预期延长。在碱性水溶液中进行Cl水解的动力学之后，进行〜195Pt NMR和HPLC分析，结果表明在这两种情况下，仅形成一种产物，PtN_3O配位球典型地具有〜195t的菌丝体位移。通过这两种方法发现的可比较的动力学数据表明，水分子在水解反应中充当亲核试剂，并且它更容易在9-甲基腺嘌呤络合物中置换Cl--配体。

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