Label-Free Electrochemiluminescence Aptasensor for 2,4,6-Trinitrotoluene Based on Bilayer Structure of Luminescence Functionalized Graphene Hybrids
Label-Free Electrochemiluminescence Aptasensor for 2,4,6-Trinitrotoluene Based on Bilayer Structure of Luminescence Functionalized Graphene Hybrids
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基于发光功能化石墨烯杂化双层结构的2,4,6-三硝基甲苯无标记电化学发光适体传感器
DOI：
10.1021/acs.analchem.5b02913
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发表时间：
2015-11-03
影响因子：
7.4
通讯作者：
Cui, Hua
中科院分区：
文献类型：
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作者：
Li, Guixin;Yu, Xinxia;Cui, Hua
用循环伏安法和脉冲电位法研究了N-氨基丁基-N-乙基异鲁米诺/氯化高氯化双官能化石墨烯杂化材料(A-H-GNS)和鲁米诺功能化银/氧化石墨烯复合材料(鲁米诺-AgNPs-GO)在循环伏安和脉冲电位下的电化学发光行为。结果表明，A-H-GNS和鲁米诺-AgNPs-GO具有良好的电致发光活性。在此基础上，基于由A-H-GNS和鲁米诺-AgNPs-GO组成的发光功能化石墨烯杂化材料的双层结构，研制了一种用于2，4，6-三硝基甲苯(TNT)检测的无标记ECL适配传感器。首先，将带正电的壳聚糖修饰的A-H-GNS修饰在掺铟氧化锡电极表面，然后将修饰后的电极浸入带负电荷的适体修饰的鲁米诺-银纳米颗粒(APTA-生物素-SA-鲁米诺-银纳米颗粒-GO)中，通过静电作用形成apta-biotin-SA-luminol-AgNPs-GO/CS-A-H-GNs/ITO电极(即适配子)。在TNT存在下，由于形成适配子TNT络合物，ECL信号显著减弱。根据TNT的抑制作用可以检测到TNT。该传感器在1.0×10~(-12)~1.0×10~(-9)g/m L范围内具有较宽的动态范围，对TNT的检测下限为6.3×10~(-13)g/m L，优于已报道的大多数生物测定方法。此外，该适配传感器已成功应用于环境水中TNT的检测。该方法灵敏、选择性强、操作简单，避免了复杂的标记和纯化过程。由于适体具有较宽的目标识别范围，这一策略为开发新的适体传感器提供了一条很有前途的途径。
The electrochemiluminescence (ECL) behavior of N-(aminobutyl)-N-(ethylisoluminol)/hemin dual-functionalized graphene hybrids (A-H-GNs) and luminol-functionalized silver/graphene oxide composite (luminol-AgNPs-GO) was investigated under cyclic voltammetry and pulse potential. It was found that A-H-GNs and luminol-AgNPs-GO exhibited excellent ECL activity. On this basis, a label-free ECL aptasensor for 2,4,6-trinitrotoluene (TNT) detection was developed based on bilayer structure of luminescence functionalized graphene hybrids consisting of A-H-GNs and luminol-AgNPs-GO. First, positively charged chitosan-coated A-H-GNs were modified on the surface of indium-doped tin oxide electrode by simple dripping and drying in the air; after that, the modified electrode was immersed in negatively charged luminol-AgNPs-GO modified with aptamer (apta-biotin-SA-luminol-AgNPs-GO) to form apta-biotin-SA-luminol-AgNPs-GO/CS-A-H-GNs/ITO electrode (i.e., aptasensor) by electrostatic interaction. In the presence of TNT, a remarkable decrease in ECL signals was observed due to the formation of aptamer TNT complex. TNT could be detected based on the inhibition effect. The aptasensor exhibits a wide dynamic range from 1.0 X 10(-12) to 1.0 X 10(-9) g/mL, with a low detection limit of 6.3 X 10(-13) g/mL for the determination of TNT, which is superior to most previously reported bioassays for TNT. Moreover, the proposed aptasensor has been successfully applied to the detection of TNT in environmental water. It is sensitive, selective, and simple, avoiding complicated labeling and purification procedures. Due to the wide target recognition range of aptamer, this strategy provides a promising way to develop new aptasensor for other analytes.