Abstract
A label-free multiplexed electrochemical biosensor based on a gold nanoparticles/graphene quantum dots/graphene oxide (AuNPs/GQDs/GO) modified three-screen-printed carbon electrode (3SPCE) array is successfully constructed to detect miRNA-21, miRNA-155, and miRNA-210 biomarkers for the first time. Redox species (anthraquinone (AQ), methylene blue (MB), and polydopamine (PDA)) are used as redox indicators for anchoring capture miRNA probes, which hybridize with the complementary targets, miRNA-21, miRNA-155, and miRNA-210, respectively. After three target miRNAs are present, the square wave voltammetry (SWV) scan displays three well-separated peaks. Each peak indicates the presence of one miRNA, and its intensity quantitatively correlates with the concentration of the corresponding target analyte. This phenomenon results in the substantial decline of the SWV peak current of the redox probes. The developed AuNPs/GQDs/GO-based biosensor reveals excellent performance for simultaneous miRNA sensing. It offers a wide linear dynamic range from 0.001 to 1000 pM with ultrasensitive low detection limits of 0.04, 0.33, and 0.28 fM for the detection of miRNA-21, miRNA-155, and miRNA-210, respectively. It also presents high selectivity and applicability for the detection of miRNAs in human serum samples. This multiplex label-free miRNA biosensor has great potential for applications in breast cancer diagnosis.
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