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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Synthesis and reactivity of a C3-symmetric trinuclear zinc(II)hydroxide catalyst efficient at phosphate diester transesterification
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Synthesis and reactivity of a C3-symmetric trinuclear zinc(II)hydroxide catalyst efficient at phosphate diester transesterification

机译：能够有效实现磷酸二酯酯交换反应的C3对称三核氢氧化锌（II）催化剂的合成与反应活性

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摘要

Inspired by trinuclear Zn(II)sites in enzymatic systems,a ligand system containing three preorganized(2-pyridyl)methyl piperazine moieties anchored onto a rigid C3-symmetric triphenoxymethane platform has been developed for preorganizing three zinc ions into an environment conducive to intramolecular interaction.Zinc(II)binding by this ligand has been analyzed by means of potentiometric measurements in 50%(v/v)CH3CN-H2O solutions.Subsequently a C3-symmetric trinuclear Zn(II)hydroxide complex of the C3-symmetric ligand was synthesized and fully characterized using NMR spectroscopy and X-ray crystallography.This complex induces a 16 900-fold rate enhancement in the catalytic cyclization of the RNA model substrate,2-hydroxypropyl-p-nitrophenyl phosphate(HPNP,pH 6.7,25°C)over the uncatalyzed reaction with multiple catalyst turnovers.The observed differences in the pH-rate profile can be attributed to the varying concentration of various trinuclear zinc species.The trinuclear Zn(II)catalyst exhibits a higher hydrolytic activity compared to its mononuclear analogue.The reactivity and structural features of this trinuclear Zn(II)complex will be discussed.
机译：受酶体系中三核Zn（II）位点的启发，开发了一种配体系统，该系统包含三个锚定在刚性C3对称三苯氧基甲烷平台上的预组织的（2-吡啶基）甲基哌嗪部分，用于将三个锌离子预组入一个有利于分子内相互作用的环境在50％（v / v）CH3CN-H2O溶液中通过电位测量法分析了该配体与锌（II）的结合，随后合成了C3对称配体的C3对称三核Zn（II）氢氧化物复合物并利用NMR光谱学和X射线晶体学对其进行了全面表征。该络合物在RNA模型底物2-羟丙基-对硝基苯基磷酸酯（HPNP，pH 6.7,25°C）的催化环化中诱导了16900倍的速率增强。在未催化反应中具有多个催化剂周转率。观察到的pH速率分布差异可归因于各种三核锌物质浓度的变化。三核Zn（II）催化剂具有比单核类似物更高的水解活性。将讨论这种三核Zn（II）配合物的反应性和结构特征。

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