College of Chemistry, Zhengzhou University, Zhengzhou, 450001, PR China.
College of Chemistry, Zhengzhou University, Zhengzhou, 450001, PR China.
Biosens Bioelectron. 2020 Jan 1;147:111759. doi: 10.1016/j.bios.2019.111759. Epub 2019 Oct 3.
Herein, a robust and highly ordered three-dimensional electrochemical DNA (3D E-DNA) biosensor was proposed, and its orientation was controlled from top down by poly adenine oligonucleotides (polyA-ODNs)-mediated rolling motor (PRM) and graftable tetrahedron DNA (GTD). The GTD with a grafting domain was immobilized on the electrode surface to construct a well-organized sensing interface and controlled the orientation and distribution of the whole system at the "bottom" of this biosensor. The polyA-ODNs regulated the direction and density of the leg DNA attached on PRM at the "top" of the biosensor. The motion was achieved through the target induced cyclic cleaving, which triggered the motor rolling rather than walk. Impressively, the duplex strand DNA (dsDNA) formed after grafting, as a girder, provided a stable support to the soft long single strand (ssDNA), which facilitated the formation of the catalytic center, elevated the efficiency of the rolling cleavage. Under the optimal conditions, the designed biosensor exhibited a lower limit of 0.17 nM and wide linear range from 0.5 nM to 1.5 μM for adenosine rapid detection. Unique dual orientation regulated characteristics of the system increased the probability hybridization enormously and improved the motion efficiency significantly, which offered new avenue of DNA nanomachines development in biosensor platform.
本文提出了一种稳健的、高度有序的三维电化学 DNA(3D E-DNA)生物传感器,并通过多聚腺嘌呤寡核苷酸(polyA-ODNs)介导的滚动马达(PRM)和可接枝四面体 DNA(GTD)自上而下控制其取向。具有接枝结构域的 GTD 固定在电极表面上,构建了一个组织良好的传感界面,并在生物传感器的“底部”控制整个系统的取向和分布。polyA-ODNs 调节附着在生物传感器“顶部”PRM 上的腿 DNA 的方向和密度。通过目标诱导的循环切割实现运动,这引发了马达的滚动而不是行走。引人注目的是,接枝后形成的双链 DNA(dsDNA)作为大梁为柔软的长单链(ssDNA)提供了稳定的支撑,这有利于催化中心的形成,提高了滚动切割的效率。在最佳条件下,设计的生物传感器对腺苷的快速检测具有较低的下限为 0.17 nM,线性范围从 0.5 nM 到 1.5 μM。该系统独特的双重取向调节特性极大地增加了杂交的概率,并显著提高了运动效率,为 DNA 纳米机器在生物传感器平台中的发展提供了新途径。