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基于电致化学发光氧化石墨烯与纳米金和适配体组装策略的 2,4,6-三硝基甲苯检测的新型均相无标记适体传感器

A novel homogeneous label-free aptasensor for 2,4,6-trinitrotoluene detection based on an assembly strategy of electrochemiluminescent graphene oxide with gold nanoparticles and aptamer.

机构信息

CAS Key Laboratory of Soft Matter Chemistry, Department of Chemistry, University of Science and Technology of China, 96 Jinzhai Road, Hefei, Anhui 230026, PR China.

出版信息

Biosens Bioelectron. 2013 May 15;43:137-42. doi: 10.1016/j.bios.2012.12.018. Epub 2012 Dec 14.

Abstract

We report a novel homogeneous label-free aptasensor for 2,4,6-trinitrotoluene (TNT) detection based on an assembly strategy of electrochemiluminescent graphene oxide (GO) with gold nanoparticles (AuNPs) and aptamer. In this sensing strategy, the anti-TNT aptamer was first assembled with AuNPs to form aptamer-AuNPs. Then ruthenium(II) complex functionalized GO (denoted as Ru-GO) was assembled with aptamer-AuNPs by electrostatic interaction. AuNPs could directly quench the electrochemiluminescence (ECL) emission of ruthenium(II) complex on the surface of Ru-GO due to the energy transfer from luminophore to the AuNPs. Weak ECL signal of the assembly was obtained. In the presence of target molecule TNT, the aptamer-AuNPs would aggregate partly due to the aptamer-target interaction and reduce quenching effect, leading to ECL signal restoration and strong ECL signal was obtained. TNT in a range of 0.01-100ngmL(-1) could be detected by use of the ECL intensity discrepancy with a low detection limit of 3.6pgmL(-1). The aptasensor also showed high selectivity towards TNT against 2,4-dinitrotoluene, p-nitrotoluene and nitrobenzene. The present aptasensor has been successfully applied to the detection of TNT in real water samples. Compared with previous reported sensors, this homogenous aptasensor avoided complicated labeling and purification procedure and showed magnificent sensitivity and high selectivity, which made it not only convenient but also time-saving and applicable. Furthermore, this sensing strategy also provides a promising way to develop new ECL aptasensor for other analytes by virtue of other aptamers.

摘要

我们报道了一种基于电化学发光氧化石墨烯(GO)与金纳米粒子(AuNPs)和适体组装策略的用于检测 2,4,6-三硝基甲苯(TNT)的新型均相无标记适体传感器。在这种传感策略中,首先将抗 TNT 适体与 AuNPs 组装形成适体-AuNPs。然后,通过静电相互作用将钌(II)配合物功能化的 GO(表示为 Ru-GO)与适体-AuNPs 组装。由于发光体向 AuNPs 的能量转移,AuNPs 可以直接猝灭 Ru-GO 表面上钌(II)配合物的电化学发光(ECL)发射。得到了微弱的组装 ECL 信号。在存在靶分子 TNT 的情况下,由于适体-靶相互作用,部分适体-AuNPs 会聚集,从而减少猝灭效应,导致 ECL 信号恢复并得到强 ECL 信号。通过使用 ECL 强度差异可以检测 0.01-100ngmL(-1) 范围内的 TNT,检测限低至 3.6pgmL(-1)。该适体传感器对 TNT 具有较高的选择性,对 2,4-二硝基甲苯、对硝基甲苯和硝基苯的选择性较高。该适体传感器已成功应用于实际水样中 TNT 的检测。与以前报道的传感器相比,这种均相适体传感器避免了复杂的标记和纯化过程,表现出了极好的灵敏度和高选择性,不仅方便而且省时、适用。此外,这种传感策略还为利用其他适体开发用于其他分析物的新型 ECL 适体传感器提供了一种有前途的方法。

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