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Efficient electrochemiluminescence quenching of carbon-coated petalous CdS nanoparticles for an ultrasensitive tumor marker assay through coreactant consumption by G-quadruplex-hemin decorated Au nanorods

机译:碳包覆的花瓣状CdS纳米粒子的高效电化学发光淬灭,用于通过G-四链体-血红素修饰的金纳米棒消耗的共反应物来进行超灵敏的肿瘤标志物测定

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摘要

A novel competitive electrochemiluminescence (ECL) aptasensor was designed for the detection of carcinoembryonic antigen (CEA) using carbon-coated petalous CdS nanopaticles (CdS-C petalous nanoparticles) as an ECL emitter and DNAzyme/Au nanorods-complementary DNA as a quenching probe. The quenching probe was firstly prepared by assembling guanine (G)-rich ssDNA and cDNA on Au nanorods and then reacting with hemin to form hemin/G-quadruplex DNAzyme units. CdS-C nanoparticles were synthesized and employed as the matrix for the construction of the CdS-C/Chit/aptamer platform. In the absence of CEA, the DNAzyme/Au nanorods as the quenching probe can be introduced by hybridization with aptamer on the surface of the sensing platform. In this state, DNAzyme immobilized on the probe catalyzes the reduction of H2O2, producing a decreased ECL emission. Upon both CEA and quenching probe addition, competitive reaction of the quenching probe and CEA with capture aptamer immobilized on the electrode occurred and thus resulted in the decreased amount of quenching probe on the electrode, which decreased the consumption of H2O2, producing an increased ECL signal. Based on this strategy, the aptasensor enables the sensitive detection of CEA in a range of 0.1 pg mL(-1) to 0.5 ng mL(-1) with a detection limit of 0.036 pg mL(-1). The limit of quantification in human serum samples was experimentally found to be 0.21 pg mL(-1). Moreover, the application of the aptasensor was demonstrated in the analysis of CEA in human serum samples with recoveries of 88.2-106%. The proposed method holds great promise in the highly sensitive and selective detection of CEA in biological samples.
机译:设计了一种新型竞争性电化学发光(ECL)适体传感器,以碳涂层的花瓣状CdS纳米颗粒(CdS-C花瓣状纳米颗粒)作为ECL发射体,并使用DNAzyme / Au纳米棒互补DNA作为淬灭探针来检测癌胚抗原(CEA)。首先通过在Au纳米棒上组装富含鸟嘌呤(G)的ssDNA和cDNA,然后与血红素反应形成血红素/ G-四链体DNA酶单位来制备淬灭探针。合成了CdS-C纳米粒子,并将其用作构建CdS-C / Chit / aptamer平台的基质。在不存在CEA的情况下,可以通过在传感平台表面上与适体杂交来引入DNAzyme / Au纳米棒作为淬灭探针。在这种状态下,固定在探针上的DNAzyme催化H2O2的减少,从而导致ECL排放降低。加入CEA和淬灭探针后,淬灭探针和CEA与固定在电极上的捕获适体发生竞争反应,从而导致电极上淬灭探针的数量减少,从而减少了H2O2的消耗,产生了增强的ECL信号。基于此策略,aptasensor可以在0.1 pg mL(-1)至0.5 ng mL(-1)的范围内灵敏检测CEA,检测极限为0.036 pg mL(-1)。通过实验发现人血清样品中的定量限为0.21 pg mL(-1)。此外,适体传感器在人体血清样品中CEA分析中的应用得到了证实,回收率为88.2-106%。该方法在生物样品中CEA的高灵敏度和选择性检测中具有广阔的前景。

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