This study reported a novel biosensor based on the nanocomposite of zirconium metal-organic framework (Zr-MOF, UiO-66) embedded with silver nanoclusters (Ag NCs) using the carcinoembryonic antigen (CEA)-targeted aptamer as template (AgNCs@Apt@UiO-66). The synthesized AgNCs@Apt@UiO-66 nanocomposite not only possesses good biocompatibility, active electrochemical performance, and strong bioaffinity, but also can be dispersed to form two-dimensional nanocomposite with nanoscale thickness. As such, the use of the AgNCs@CEA-aptamer enables AgNC@Apt@UiO-66 with sensitive and selective detection capacity of trace CEA, further concurrently being exploited as scaffold for surface plasmon resonance spectroscopy (SPR) and electrochemical biosensors. The results showed that the proposed electrochemical AgNC@Apt@UiO-66-based aptasensor exhibits high sensitivity with a low detection limit (LOD) of 8.88 and 4.93 pg·mL deduced from electrochemical impedance spectroscopy and differential pulse voltammetry, respectively, within a broad linear range of the CEA concentration (0.01-10 ng·mL). Meanwhile, the developed SPR biosensor exhibited a slightly high LOD of 0.3 ng·mL within the CEA concentration of 1.0-250 ng·mL. Both the electrochemical and SPR aptasensors displayed high selectivity, good reproducibility, stability, acceptable regenerability, and applicability in real human serum samples. These results proved that the proposed aptamer-targeted Zr-MOF nanocomposite can be utilized in multiple-functionally biosensing, further promoting the potential application of Zr-MOF-related nanomaterials in clinical diagnosis.

Two-dimensional (2D) zirconium-based metal-organic framework nanosheets embedded with Au nanoclusters (denoted as 2D AuNCs@521-MOF) were prepared via a one-pot method under mild conditions. The optimized 2D AuNCs@521-MOF nanosheets not only possessed high specific surface area, physicochemical stability, and good electrochemical activity but also exhibited strong bioaffinity toward biomolecule-bearing phosphate groups. Consequently, a large amount of cocaine aptamer strands can be immobilized onto the substrate modified by 2D AuNCs@521-MOF nanosheet, further leading to the formation of a constructed biosensitive platform, which can be used to successfully detect cocaine through the specific binding interactions between cocaine and aptamer strands. The results demonstrated that the 2D AuNCs@521-MOF-based aptasensor had high sensitivity for detecting cocaine within the broad concentration range of 0.001-1.0 ng·mL and the low limit of detection of 1.29 pM (0.44 pg·mL) and 2.22 pM (0.75 pg·mL) as determined by electrochemical impedance spectroscopy and differential pulse voltammetry, respectively. As expected, with the advantages of high selectivity, repeatability, stability, and simple operation, this new strategy is believed to exhibit great potential for simple and convenient detection of cocaine.

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