Quadrilateral Nucleic Acid Frame-Accelerating DNAzyme Walker Kinetics for Biosensing Based on Host–Guest Recognition-Enhanced Electrochemiluminescence
Quadrilateral Nucleic Acid Frame-Accelerating DNAzyme Walker Kinetics for Biosensing Based on Host–Guest Recognition-Enhanced Electrochemiluminescence
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基于宿主-客体识别增强电化学发光的四边形核酸框架加速 DNAzyme Walker 动力学用于生物传感
DOI：
10.1021/acs.analchem.1c03525
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发表时间：
2021
影响因子：
7.4
通讯作者：
Ruo Yuan
中科院分区：
文献类型：
--
作者：
Fang Yang;Jia-Shuang Yao;Shu-Chun Bu;Hua-Ying Meng;Ying Zhuo;Xia Zhong;Ruo Yuan
DNA步行器依靠步行器和轨迹之间的反应，能够连续输出信号，这引起了生物分析界的极大关注。因此，如何改进其反应动力学以实现高效的信号读出具有重要的意义。本文通过将一个步行器和三个DNA轨迹共定位在四边形的核酸框架中，形成一个反应单元(简称qDNA步行器)，从而构建了一个四边形DNAzyme步行器。令人印象深刻的是，与普通的游离DNAzyme Walker相比，qDNA Walker的反应动力学速度快了2.3倍，可以在30分钟内实现microRNA的检测。同时，基于南瓜脲(CB，主体分子)和蒽(Ant，客体分子)的自组装，得到了一种基于蒽-葫芦巴超分子纳米晶(Ant-CB SNCs)的电致化学发光(ECL)发射体。得益于主客体识别效应，制备的Ant-CB SNCs由于CB与Ant之间的超分子相互作用而提高了ECL效率，从而抑制了Ant分子的振动和旋转。我们将这种新的增强型ECL现象定义为“主-客识别-增强型ECL”。作为概念验证，将高效的DNAzyme步行器和Ant-CB SNCs先进的ECL发射器相结合，构建了针对microRNA-21的ECL生物传感器(miRNA-21)，该传感器在50~50 PM之间呈线性关系，低检测限(11 Am)，突出了其在临床诊断中的巨大潜力。
Depending on the reaction between walkers and tracks, DNA walker is able to output signals continuously, which has attracted great attention from the bioanalytical community. Therefore, how to improve its reaction kinetics for efficient signal readout is of great significance. Herein, a quadrilateral DNAzyme walker was fabricated by colocalizing one walker and three DNA tracks in the quadrilateral nucleic acid frame to form a reaction unit (abbreviated as qDNA walker). Impressively, in contrast to the common free DNAzyme walker, the reaction kinetics of the qDNA walker was 2.3 times faster, which could achieve microRNA detection within 30 min. Meanwhile, an electrochemiluminescence (ECL) emitter of anthracene–cucurbituril supramolecular nanocrystals (Ant–CB SNCs) was obtained based on the self-assembly of cucurbituril (CB, host molecule) and anthracene (Ant, guest molecule). Benefiting from the host–guest recognition effect, the prepared Ant–CB SNCs exhibited enhanced ECL efficiency due to the supramolecular interaction between CB and Ant, which could inhibit vibration and rotation of the Ant molecules. We defined this new enhanced ECL phenomenon as “host–guest recognition-enhanced ECL.” As a proof of concept, an ECL biosensor for microRNA-21 (miRNA-21) was constructed by combining the high-efficiency DNAzyme walker and the advanced ECL emitter of Ant–CB SNCs, which showed a linear range from 50 aM to 50 pM with a low limit of detection (11 aM), highlighting the great potential in clinical diagnosis.