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A sensitive sandwich electrochemiluminescence immunosensor was established by employing graphene oxide-PEI-carbon quantum dots (CQDs)-Au nanohybrid as probe to measure carbohydrate antigen 15-3 (CA15-3), a breast cancer biomarker. In this work, nanocomposites of Ag nanoparticles and polydopamine (AgNPs-PDA) were synthesized by redox reaction between dopamine and Ag+. The nanocomposite with high surface area can provide an efficient substrate for immobilizing initial antibody (Ab1). Carbon quantum dots (CQDs) are fixed on polyethylenimine-functionalized graphene oxide (PEI-GO) by amide bonds. Au nanoparticles are modified on CQDs-decorated PEI-GO substrates. The secondary antibody (Ab2) was immobilized by AuNPs/CQDs-PEI-GO composite. CQDs can be assembled onto the surface of an electrode by incorporation of CA15-3 with Ab1 and Ab2. Under the synergistic action of AgNPs, polydopamine, AuNPs, and PEI-GO, the ECL signal of CQDs is greatly amplified as an excellent conductive material to facilitate electron transfer rate and further increase electrochemical detection capability. Under optimal conditions, the fabricated immunosensor showed a linear concentration range from 0.005 to 500 U mL–1, with a detection limit of 0.0017 U mL–1 (signal-to-noise ratio of 3) for CA15-3. The designed ECL immunosensor displayed receivable accuracy, excellent stability, and high specificity. The results of the detection of human serum samples are satisfactory, revealing that the method offers a potential application for the clinical diagnosis of tumor markers.

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A hydrothermal strategy for preparing boron and nitrogen codoped carbon quantum dots was studied using the precursors of p-amino salicylic acid, boric acid and ethylene glycol dimethacrylate. The boron and nitrogen codoped carbon quantum dots have high fluorescence intensity, good monodispersity, high stability, superior water solubility, and a fluorescence quantum yield of 19.6%. Their average size is 5 nm. Their maximum excitation and emission wavelengths are 380 and 520 nm, respectively. Permanganate (MnO 4 − ) quenched boron and nitrogen codoped carbon quantum dots fluorescence through inner filter effect and static quenching effects. The linear relation between quenching efficiency and MnO 4 − concentration ranged from 0.05 to 60 μmol/L with a detection limit of 13 nmol/L. In the presence of captopril, MnO 4 − was reduced to Mn 2+ and the fluorescence of boron and nitrogen codoped carbon quantum dots was recovered. The linear range between recovery and captopril concentration was from 0.1 to 60 μmol/L. The limit of detection was 0.03 μmol/L. The developed method can be employed as a sensitive fluorescence sensing platform for MnO 4 − . It has been successfully used for captopril detection in mouse plasma.

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