Zhou Qian, Lin Youxiu, Lu Minghua, Tang Dianping
Key Laboratory of Analytic Science for Food Safety and Biology (MOE & Fujian Province), State Key Laboratory of Photocatalysis on Energy and Environment, Collaborative Innovation Center of Detection Technology for Haixi Food Safety and Products (Fujian Province), Department of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China.
J Mater Chem B. 2017 Dec 28;5(48):9600-9607. doi: 10.1039/c7tb02354e. Epub 2017 Dec 4.
This work designs a new photoelectrochemical (PEC) sensing system for the detection of carcinoembryonic antigens (CEAs) using bismuth ferrite (BiFeO) nanostructures as photoactive materials, accompanied by the target-controlled release of glucose from multifunctional mesoporous silica nanoparticles (MSNs) for signal amplification. Glucose molecules were gated in the pores via the hybridization of a CEA aptamer with anchor DNA (aDNA, modified on the mesoporous silica nanoparticles). Upon the addition of the target CEA, the analyte competitively reacted with the aptamer to open the gate, thus resulting in the release of glucose molecules from the MSNs. Based on the oxidization of glucose in the presence of glucose oxidase, the as-generated enzymatic product (HO) served as an electron acceptor to enhance the photocurrent generated by the BiFeO nanostructures under visible light irradiation. In this way, an in situ amplified photocurrent could be achieved in that the low-concentration target CEA could cause the release of numerous glucose molecules. Experimental results suggested that the photocurrent obtained from the BiFeO-based photoactive materials increased with increasing CEA concentration and showed a good linear dependence on the logarithm of the CEA level from 5.0 pg mL to 50 ng mL under optimal conditions. Additionally, the BiFeO-based PEC sensing platform also showed good stability and favorable selectivity, and satisfactory accuracy for CEA detection in human serum specimens in comparison with a reference CEA ELISA kit. The good analytical performance of the BiFeO-based PEC sensing method makes it a promising tool for the efficient, low-cost and convenient detection of CEAs in disease diagnosis.
本研究设计了一种新型光电化学(PEC)传感系统,用于检测癌胚抗原(CEA),该系统使用铁酸铋(BiFeO)纳米结构作为光活性材料,并通过多功能介孔二氧化硅纳米颗粒(MSN)实现葡萄糖的目标控制释放以进行信号放大。葡萄糖分子通过CEA适配体与锚定DNA(aDNA,修饰在介孔二氧化硅纳米颗粒上)的杂交被封闭在孔中。加入目标CEA后,分析物与适配体竞争性反应打开通道,从而导致葡萄糖分子从MSN中释放出来。基于葡萄糖在葡萄糖氧化酶存在下的氧化反应,生成的酶产物(H₂O₂)作为电子受体,增强了BiFeO纳米结构在可见光照射下产生的光电流。通过这种方式,低浓度的目标CEA可导致大量葡萄糖分子的释放,从而实现原位光电流放大。实验结果表明,基于BiFeO的光活性材料获得的光电流随CEA浓度的增加而增加,在最佳条件下,对5.0 pg/mL至50 ng/mL的CEA水平对数呈良好的线性依赖关系。此外,基于BiFeO的PEC传感平台还表现出良好的稳定性和选择性,与参考CEA ELISA试剂盒相比,对人血清样本中的CEA检测具有令人满意的准确性。基于BiFeO的PEC传感方法良好的分析性能使其成为疾病诊断中高效、低成本且便捷检测CEA的有前途的工具。