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通过聚腺嘌呤辅助的表面增强拉曼散射硅芯片对实际体系中铅离子进行超灵敏、特异性、可回收及可重现的检测。

Ultrasensitive, Specific, Recyclable, and Reproducible Detection of Lead Ions in Real Systems through a Polyadenine-Assisted, Surface-Enhanced Raman Scattering Silicon Chip.

作者信息

Shi Yu, Wang Houyu, Jiang Xiangxu, Sun Bin, Song Bin, Su Yuanyuan, He Yao

机构信息

Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Institute of Functional Nano and Soft Materials (FUNSOM), Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University , Suzhou, Jiangsu 215123, China.

出版信息

Anal Chem. 2016 Apr 5;88(7):3723-9. doi: 10.1021/acs.analchem.5b04551. Epub 2016 Mar 9.

DOI:10.1021/acs.analchem.5b04551
PMID:26923545
Abstract

It is of great significance to accurately and reliably detect trace lead(II) (Pb(2+)) ions, preferably at sub-nM level due to the possible long-term accumulation of Pb(2+) in the human body, which may cause serious threats to human health. However, a suitable Pb(2+) sensor meeting the demands is still scanty. Herein, we develop a polyadenine-assisted, surface-enhanced Raman scattering (SERS) silicon chip (0.5 cm × 0.5 cm) composed of core (Ag)-satellite (Au) nanoparticles (Ag-Au NPs)-decorated silicon wafers (Ag-Au NPs@Si) for high-performance Pb(2+) detection. Typically, strong SERS signals could be measured when DNAzyme conjugated on the SERS silicon chip is specifically activated by Pb(2+), cleaving the substrate strand into two free DNA strands. A good linearity exists between the normalized Raman intensities and the logarithmic concentrations of Pb(2+) ranging from 10 pM to 1 μM with a good correlation coefficient, R(2) of 0.997. Remarkably, Pb(2+) ions with a low concentration of 8.9 × 10(-12) M can be readily determined via the SERS silicon chip ascribed to its superior SERS enhancement, much lower than those (∼nM) reported by other SERS sensors. Additionally, the developed chip features good selectivity and recyclability (e.g., ∼11.1% loss of Raman intensity after three cycles). More importantly, the as-prepared chip can be used for accurate and reliable determination of unknown Pb(2+) ions in real systems including lake water, tap water and industrial wastewater, with the RSD value less than 12%.

摘要

准确可靠地检测痕量铅离子(Pb(2+))具有重要意义。由于Pb(2+)可能在人体中长期积累,对人体健康造成严重威胁,因此最好能在亚纳摩尔水平进行检测。然而,满足这一需求的合适的Pb(2+)传感器仍然很少。在此,我们开发了一种由核(Ag)-卫星(Au)纳米颗粒(Ag-Au NPs)修饰的硅片(Ag-Au NPs@Si)组成的聚腺嘌呤辅助表面增强拉曼散射(SERS)硅芯片(0.5 cm×0.5 cm),用于高性能的Pb(2+)检测。通常,当SERS硅芯片上共轭的DNAzyme被Pb(2+)特异性激活,将底物链切割成两条游离DNA链时,可以测量到强烈的SERS信号。在10 pM至1 μM的Pb(2+)对数浓度与归一化拉曼强度之间存在良好的线性关系,相关系数R(2)为0.997。值得注意的是,由于其优异的SERS增强性能,低至8.9×10(-12) M的Pb(2+)离子可以通过SERS硅芯片轻松测定,这比其他SERS传感器报道的浓度(~nM)低得多。此外,所开发的芯片具有良好的选择性和可回收性(例如,三个循环后拉曼强度损失约11.1%)。更重要的是,所制备的芯片可用于准确可靠地测定包括湖水、自来水和工业废水在内的实际系统中的未知Pb(2+)离子,相对标准偏差(RSD)值小于12%。

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