Cu(II)-mediated stabilisation of DNA duplexes bearing consecutive ethenoadenine lesions and its application to a metal-responsive DNAzyme
Cu(II)-mediated stabilisation of DNA duplexes bearing consecutive ethenoadenine lesions and its application to a metal-responsive DNAzyme
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Cu(II) 介导的带有连续乙烯腺嘌呤损伤的 DNA 双链体的稳定及其在金属响应 DNAzyme 中的应用
DOI：
10.1039/d2cc06179a
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发表时间：
2023
影响因子：
4.9
通讯作者：
Mitsuhiko Shionoya
中科院分区：
文献类型：
--
作者：
Silpa Chandran Rajasree;Yusuke Takezawa;Mitsuhiko Shionoya
金属介导的核碱基配对可以在金属响应DNA功能的表达中发挥核心作用。我们报告了CuII介导的DNA双链体的稳定性，其带有受损的核碱基，1，N6-乙烯基腺嘌呤（εA）作为金属结合位点，用于构建金属响应性DNA酶。连续掺入三个或更多个εA-εA错配对允许通过金属介导的ε A-Cu II-εA碱基配对实现Cu II依赖性显著双链体稳定。随后，策略性地设计了具有三个ε A-Cu II-εA碱基对的分裂DNA酶。加入CuII离子后，ε A修饰的DNAzyme的活性提高了5.3倍。这项研究证明了εA损伤对于构建金属响应DNA架构的实用性。
Metal-mediated nucleobase pairing can play a central role in the expression of metal-responsive DNA functions. We report the CuII-mediated stabilisation of DNA duplexes bearing damaged nucleobases, 1,N6-ethenoadenine (εA), as metal-binding sites, which was utilised to construct a metal-responsive DNAzyme. Consecutive incorporation of three or more εA–εA mismatch pairs allowed for CuII-dependent significant duplex stabilisation through metal-mediated εA–CuII–εA base pairing. Subsequently, a split DNAzyme with three εA–CuII–εA base pairs was strategically designed. The activity of the εA-modified DNAzyme was enhanced by 5.3-fold upon addition of CuII ions. This study demonstrates the utility of εA lesions for building metal-responsive DNA architectures.