Sharp Switching of DNAzyme Activity through the Formation of a CuII -Mediated Carboxyimidazole Base Pair.,Angewandte Chemie International Edition

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Sharp Switching of DNAzyme Activity through the Formation of a CuII -Mediated Carboxyimidazole Base Pair.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-08-10 , DOI: 10.1002/anie.202009579
Yusuke Takezawa ₁ , Lingyun Hu ₁ , Takahiro Nakama ₁ , Mitsuhiko Shionoya ₁

Affiliation

DNAzymes are widely used as functional units for creating DNA‐based sensors and devices. Switching of DNAzyme activity by external stimuli is of increasing interest. Herein we report a Cu^II‐responsive DNAzyme rationally designed by incorporating one of the most stabilizing artificial metallo‐base pairs, a Cu^II‐mediated carboxyimidazole base pair (Im^C‐Cu^II‐Im^C), into a known RNA‐cleaving DNAzyme. Cleavage of the substrate was suppressed without Cu^II, but the reaction proceeded efficiently in the presence of Cu^II ions. This is due to the induction of a catalytically active structure by Im^C‐Cu^II‐Im^C pairing. The on/off ratio was as high as 12‐fold, which far exceeds that of the previously reported DNAzyme with a Cu^II‐mediated hydroxypyridone base pair. The DNAzyme activity can be regulated specifically in response to Cu^II ions during the reaction through the addition, removal, or reduction of Cu^II. This approach should advance the development of stimuli‐responsive DNA systems with a well‐defined sharp switching function.

中文翻译：

通过形成CuII介导的羧咪唑碱基对，DNA酶活性急剧变化。

DNAzyme被广泛用作创建基于DNA的传感器和设备的功能单元。外部刺激对DNAzyme活性的转换引起了越来越多的关注。本文我们报告一个的Cu ^II响应性DNA核酶合理通过将最稳定人工金属-碱基对中的一个设计中，铜^II介导的carboxyimidazole碱基对（IM ^ç -Cu ^II -Im ^Ç），进入一个已知的RNA切割核酶。在没有Cu ^II的情况下抑制了基体的裂解，但是在Cu ^II离子的存在下反应有效地进行了。这是由于Im ^C ‐Cu ^II ‐Im诱导了催化活性结构^C配对。开/关比高达12倍，远远超过了先前报道的带有Cu ^II介导的羟基吡啶酮碱基对的DNAzyme。通过添加，去除或还原Cu ^II，可以在反应过程中响应Cu ^II离子来具体调节DNAzyme的活性。这种方法应促进具有明确定义的快速切换功能的刺激响应性DNA系统的开发。

更新日期：2020-08-10

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