Browsing by Author "Adeniyi, Kayode Omotayo"

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    Molecularly Imprinted Viral Protein Integrated Zn–Cu–In–Se–P Quantum Dots Superlattice for Quantitative Ratiometric Electrochemical Detection of SARS-CoV-2 Spike Protein in Saliva
    (American Chemical Society , 2024-08-09) Adeniyi, Kayode Omotayo; Oyinlola, Kayode; Achadu, Ojodomo J; Menard, Herve; Grillo, Federico; Yang, Zhugen; Adegoke, Oluwasesan
    Solution-processable colloidal quantum dots (QDs) are promising materials for the development of rapid and low-cost, next-generation quantum-sensing diagnostic systems. In this study, we report on the synthesis of multinary Zn-Cu-In-Se-P (ZCISeP) QDs and the application of the QDs-modified electrode (QDs/SPCE) as a solid superlattice transducer interface for the ratiometric electrochemical detection of the SARS-CoV-2-S1 protein in saliva. The ZCISeP QDs were synthesized through the formation of In(Zn)PSe QDs from InP QDs, followed by the incorporation of Cu cations into the crystal lattice via cation exchange processes. A viral-protein-imprinted polymer film was deposited onto the QDs/SPCE for the specific binding of SARS-CoV-2. Molecular imprinting of the virus protein was achieved using a surface imprinting electropolymerization strategy to create the MIP@QDs/SPCE nanosensor. Characterization through spectroscopic, microscopic, and electrochemical techniques confirmed the structural properties and electronic-band state of the ZCISeP QDs. Cyclic voltammetry studies of the QDs/SPCE superlattice confirmed efficient electron transport properties and revealed an intraband gap energy state with redox peaks attributed to the Cu1+/2+ defects. Binding of SARS-CoV-2-S1 to the MIP@QDs/SPCE cavities induced a gating effect that modulated the Fe(CN)63-/4- and Cu1+/2+ redox processes at the nanosensor interface, producing dual off/on ratiometric electrical current signals. Under optimal assay conditions, the nanosensor exhibited a wide linear detection range (0.001-100 pg/mL) and a low detection limit (0.34 pg/mL, 4.6 fM) for quantitative detection of SARS-CoV-2-S1 in saliva. The MIP@QDs/SPCE nanosensor demonstrated excellent selectivity against nonspecific protein targets, and the integration with a smartphone-based potentiostat confirmed the potential for point-of-care applications.
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    An organic-inorganic polyacrylamide-based surface imprinted quantum dots for the impedimetric and voltammetric detection of diazepam in saliva with smartphone readout
    (Elsevier, 2025-04-01) Adegoke, Oluwasesan; Oyinlola, Kayode; Adeniyi, Kayode Omotayo; Achadu, Ojodomo J; Yang, Zhugen; Daeid, Niamh Nic
    Diazepam (DZP) is a muscle-relaxing, anxiety-relieving sedative drug; nonetheless, it is also an addictive drug that may be abused. This work reports on the development of a novel electrochemical nanosensor for diazepam using SiO2-encapsulated-3-mercaptopropionic acid-capped AuZnCeSeS quantum dots (QDs) overcoated with a molecularly imprinted polymer (MIP) on screen-printed carbon electrodes (SPCEs). Electrochemical, spectroscopic and electron microscopic characterization of the nanomaterial and modified electrode surface was carried out and is reported herein. Specifically, electrochemical characterization of the QDs/SPCE using cyclic voltammetry (CV) revealed that the QDs exhibit a higher electrode surface area whilst electrochemical impedance spectroscopy (EIS) characterization demonstrated a lower charge transfer resistance (Rct). To fabricate the electrochemical nanosensor, firstly, alloyed AuZnCeSeS QDs were synthesized in the organic phase and thereafter capped with 3-mercaptopropionic acid (MPA) via a ligand exchange reaction. The MPA-AuZnCeSeS QDs were encapsulated in a SiO2 layer to form a SiO2-MPA AuZnCeSeS QDs system. The QDs were drop-casted onto SPCEs to form a SiO2-MPA AuZnCeSeS QDs/SPCE transducer interface. Organic based acrylamide, used as a functional monomer, was electropolymerized via CV on the QDs/SPCE in the presence of the diazepam template with ethylene glycol dimethacrylate as a crosslinker and 2,2′-azobis(2-methylpropionitrile) as an initiator. Under optimum experimental conditions, DZP was detected using EIS and square wave voltammetry (SWV). Using a portable potentiostat and a hand-held smartphone-based potentiostat, DZP was quantitatively detected in saliva using the MIP@QDs/SPCE with a limit of detection (LOD) of 2.3 μM and 2.7 μM, respectively. The LOD for DZP from SWV analysis was 1.0 μM.