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首页> 外文期刊>Chemistry: A European journal >Preorganized Bis-Zinc Phosphodiester Cleavage Catalysts Possessing Natural Ligands: A Lesson Pertinent to Bimetallic Artificial Enzymes
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Preorganized Bis-Zinc Phosphodiester Cleavage Catalysts Possessing Natural Ligands: A Lesson Pertinent to Bimetallic Artificial Enzymes

机译：具有天然配体的预组织的双锌磷酸二酯裂解催化剂：与双金属人工酶有关的一课

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摘要

Two preorganized bis-zinc recetpors (2 and 3) were synthesized wherein the metals were ligated with ligands present in natural phosphodiesterases: imidazoles and carboxylates. The intrametallic distance is near 4.5 A, that found in natural nucleases and other successful artificial nucleases. With only two imidazoles (2), the zinc binding affinities were not high enough to achieve cooperativity. Yet, with a third ligand, a carboxylate (3), cooperativity was found in the cleavage of HPNPP. The preorganization of 3 was achieved uisng a "steric gearing" strategy. The enhancement was 80-fold for cooperation between the two metals relative to a mono-metallic analogue (5). However, there was no observable enhancement in the hydrolysis of RNA using 3 relative to 5. Therefore, we conclude that placing two zinc atoms that are ligated with natural ligands at the appropriate distance for catalysis is not sufficient to enhance the cleavage of RNA, but is successful for activated RNA substrate mimics.
机译：合成了两个预组织的双锌酯（2和3），其中金属与天然磷酸二酯酶中存在的配体连接：咪唑和羧酸酯。金属内距离接近4.5 A，这是在天然核酸酶和其他成功的人工核酸酶中发现的。仅使用两个咪唑（2），锌结合亲和力不足以实现协同作用。然而，对于第三种配体，即羧酸盐（3），在HPNPP的裂解中发现了协同作用。 3的预组织是通过“空间齿轮”策略实现的。相对于单金属类似物（5），两种金属之间的配合提高了80倍。但是，相对于5，使用3时，RNA的水解没有可观察到的增强。因此，我们得出结论，将与天然配体连接的两个锌原子置于适当的距离进行催化不足以增强RNA的裂解，但是对于活化的RNA底物模拟物是成功的。

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