ATP-Responsive Strand Displacement Coupling with DNA Origami/AuNPs Strategy for the Determination of Microcystin-LR Using Surface-Enhanced Raman Spectroscopy.
ATP-Responsive Strand Displacement Coupling with DNA Origami/AuNPs Strategy for the Determination of Microcystin-LR Using Surface-Enhanced Raman Spectroscopy.
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DOI：
10.1021/acs.analchem.2c02440
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发表时间：
2022-08
影响因子：
7.4
通讯作者：
Bingyang Huo;Ling Xia;Zhixian Gao;Gongke Li;Yuling Hu
中科院分区：
文献类型：
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作者：
Bingyang Huo;Ling Xia;Zhixian Gao;Gongke Li;Yuling Hu
DNA折纸介导的自组装策略已成为表面增强拉曼光谱（Sers）的有力工具。然而，这些自组装方法通常不具有高检测特异性。本文提出了一种基于三磷酸腺苷（ATP）响应链置换（ARSD）与DNA折纸/金纳米粒子偶联的微囊藻毒素-LR（MC-LR）表面增强拉曼光谱（Sers）分析的新方法。在MC-LR和ATP分子的存在下，用抗MC-LR适体（T1）和ATP适体（T2）制造的核酸传感结构被触发以释放剩余的ATP。此外，DNA折纸辅助组装导致形成均匀的等离子体纳米结构，用于通过强等离子体耦合的拉曼增强。在功能化DNA折纸/AuNP的间隙中结合后，ATP分子的拉曼位移变得可检测，导致734 cm-1处的Sers强度增加。MC-LR在1.56 ~ 50 μg·L-1范围内线性关系良好，检出限为0.29 μg·L-1。结合固相萃取样品预处理提取和10倍浓缩，该方法成功用于真实的湖水样品中MC-LR型的检测，回收率为98.4 ~ 116%，相对标准偏差为1.9- 6.7%.此外，用于检测污染湖水样品中的MC-LR，所开发的方法和超高效液相色谱-串联质谱法的结果被发现是一致的，相对误差在-12%至2.4%之间。所提出的策略为痕量MC-LR分析提供了灵敏的识别和信号放大平台，并且更普遍地为毒素分析提供了创新的核酸传感结构。
The DNA origami-mediated self-assembly strategy has emerged as a powerful tool in surface-enhanced Raman spectroscopy (SERS). However, these self-assembly approaches typically do not possess high detection specificity. Herein, a novel strategy based on adenosine triphosphate (ATP)-responsive strand displacement (ARSD) coupling with DNA origami/AuNPs for SERS analysis of microcystin-LR (MC-LR) is presented. In the presence of MC-LR and ATP molecules, nucleic acid sensing structures fabricated with anti-MC-LR aptamer (T1) and ATP aptamer (T2) were triggered to release the remaining ATP. In addition, DNA origami-assisted assembly results in the formation of homogeneous plasmonic nanostructures for Raman enhancement via strong plasmonic coupling. After the binding in the gaps of functionalized DNA origami/AuNPs, the Raman shift of the ATP molecules becomes detectable, leading to increased SERS intensity in 734 cm-1. A linear response to MC-LR was obtained in the concentration range of 1.56-50 μg·L-1, and the limit of detection (LOD) was 0.29 μg·L-1. Combined with the solid-phase extraction sample pretreatment for extraction and 10-fold concentration, this proposed method was successfully used to detect MC-LR type in real lake-water samples with good recoveries of 98.4-116% and relative standard deviations of 1.9-6.7%. Furthermore, for the detection of MC-LR in contaminated lake-water samples, the results of the developed method and ultrahigh-performance liquid chromatography-tandem mass spectrometry were found to be in agreement with relative errors between -12 and 2.4%. The proposed strategy provides a sensitive recognition and signal amplification platform for trace MC-LR analysis as well as innovative nucleic acid sensing structures for toxin analysis more generally.