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ATP-Responsive Strand Displacement Coupling with DNA Origami/AuNPs Strategy for the Determination of Microcystin-LR Using Surface-Enhanced Raman Spectroscopy
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-08-16 , DOI: 10.1021/acs.analchem.2c02440
Bingyang Huo 1 , Ling Xia 1 , Zhixian Gao 2 , Gongke Li 1 , Yuling Hu 1
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-08-16 , DOI: 10.1021/acs.analchem.2c02440
Bingyang Huo 1 , Ling Xia 1 , Zhixian Gao 2 , Gongke Li 1 , Yuling Hu 1
Affiliation
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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.
中文翻译：
ATP 响应链置换偶联与 DNA 折纸/AuNPs 策略使用表面增强拉曼光谱测定微囊藻毒素-LR
DNA 折纸介导的自组装策略已成为表面增强拉曼光谱 (SERS) 中的强大工具。然而，这些自组装方法通常不具备高检测特异性。在此，提出了一种基于三磷酸腺苷 (ATP) 响应链置换 (ARSD) 与 DNA 折纸/AuNPs 耦合的新策略，用于微囊藻毒素-LR (MC-LR) 的 SERS 分析。在存在 MC-LR 和 ATP 分子的情况下，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折纸辅助组装导致通过强等离子体耦合形成用于拉曼增强的均匀等离子体纳米结构。在功能化 DNA 折纸/AuNPs 的间隙中结合后，–1。MC-LR 在 1.56–50 μg·L –1的浓度范围内得到线性响应，检测限 (LOD) 为 0.29 μg·L –1. 结合固相萃取样品预处理提取和10倍浓缩，该方法成功用于检测真实湖水样品中的MC-LR型，良好的回收率为98.4-116%，相对标准偏差为1.9- 6.7%。此外，对于污染湖水样品中 MC-LR 的检测，发现所开发方法和超高效液相色谱 - 串联质谱的结果与 -12 和 2.4% 之间的相对误差一致。所提出的策略为痕量 MC-LR 分析提供了一个灵敏的识别和信号放大平台，并为更普遍的毒素分析提供了创新的核酸传感结构。
更新日期：2022-08-16
中文翻译：
ATP 响应链置换偶联与 DNA 折纸/AuNPs 策略使用表面增强拉曼光谱测定微囊藻毒素-LR
DNA 折纸介导的自组装策略已成为表面增强拉曼光谱 (SERS) 中的强大工具。然而，这些自组装方法通常不具备高检测特异性。在此，提出了一种基于三磷酸腺苷 (ATP) 响应链置换 (ARSD) 与 DNA 折纸/AuNPs 耦合的新策略，用于微囊藻毒素-LR (MC-LR) 的 SERS 分析。在存在 MC-LR 和 ATP 分子的情况下，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折纸辅助组装导致通过强等离子体耦合形成用于拉曼增强的均匀等离子体纳米结构。在功能化 DNA 折纸/AuNPs 的间隙中结合后，–1。MC-LR 在 1.56–50 μg·L –1的浓度范围内得到线性响应，检测限 (LOD) 为 0.29 μg·L –1. 结合固相萃取样品预处理提取和10倍浓缩，该方法成功用于检测真实湖水样品中的MC-LR型，良好的回收率为98.4-116%，相对标准偏差为1.9- 6.7%。此外，对于污染湖水样品中 MC-LR 的检测，发现所开发方法和超高效液相色谱 - 串联质谱的结果与 -12 和 2.4% 之间的相对误差一致。所提出的策略为痕量 MC-LR 分析提供了一个灵敏的识别和信号放大平台，并为更普遍的毒素分析提供了创新的核酸传感结构。
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