Amino-functionalized vertically ordered mesoporous silica film on electrochemically polarized screen-printed carbon electrodes for the construction of gated electrochemical aptasensors and sensitive detection of carcinoembryonic antigens

在电化学极化丝网印刷碳电极上制备氨基功能化垂直有序介孔二氧化硅薄膜,用于构建门控电化学适体传感器和灵敏检测癌胚抗原

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Abstract

Disposable electrochemical biosensors with high sensitivity are very fit for point-of-care testing in clinical diagnosis. Herein, amino-functionalized, vertically ordered mesoporous silica films (NH(2)-VMSF) attached to an electrochemically polarized screen-printed carbon electrode (p-SPCE) are prepared using a simple electrochemical method and then utilized to construct a gated electrochemical aptasensor for rapid and sensitive determination of carcinoembryonic antigen (CEA). After being treated with the electrochemical polarization procedure, p-SPCE has plentiful oxygen-containing groups and improved catalytic ability, which help promote the stability of NH(2)-VMSF on SPCE without the use of an adhesive layer and simultaneously generate a highly electroactive sensing interface. Owing to the numerous uniform and ultrasmall nanopores of NH(2)-VMSF, CEA-specific aptamer anchored on the external surface of NH(2)-VMSF/p-SPCE serves as the gatekeeper, allowing the specific recognition and binding of CEA and eventually impeding the ingress of electrochemical probes [Fe(CN)(6) (3-/4-)] through the silica nanochannels. The declined electrochemical responses of Fe(CN)(6) (3-/4-) can be used to quantitatively detect CEA, yielding a wide detection range (100 fg/mL to 100 ng/mL) and a low limit of detection (24 fg/mL). Moreover, the proposed NH(2)-VMSF/p-SPCE-based electrochemical aptasensor can be applied to detect the amount of CEA in spiked human serum samples, which extends the biological application of a disposable NH(2)-VMSF/p-SPCE sensor by modulating the biological recognition species.

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