Abstract
Hydroxyurea, an oral medication with important clinical benefits in the treatment of sickle cell anemia, can be accurately determined in plasma with a transition metal dichalcogenide-based electrochemical sensor. We used a two-dimensional molybdenum sulfide material (MoS2) selectively electrodeposited on a polycrystalline gold electrode via tailored waveform polarization in the gold electrical double layer formation region. The electro-activity of the modified electrode depends on the electrical waveform parameters used to electro-deposit MoS2. The concomitant oxidation of the MoS2 material during its electrodeposition allows for the tuning of the sensor’s specificity. Chemometrics, utilizing mathematical procedures such as principal component analysis and multivariable partial least square regression, were used to process the electrochemical data generated at the bare and the modified electrodes, thus allowing the hydroxyurea concentrations to be predicted in human plasma. A limit-of-detection of 22 nM and a sensitivity of 37 nA cm−2 µM−1 were found to be suitable for pharmaceutical and clinical applications.
Highlights
Sickle cell anemia is a common inherited blood disorder that leads to major morbidity and early mortality [1,2,3,4]
Electrodeposition of MoS2 allows for the fine-tuning of the faradaic and capacitive properties of the TMDCmodified electrode, which is possible with a tailored waveform polarization (Figure 1b)
The MoS2 material was electrodeposited with cyclic voltammetry (CV), as reported earlier (Figure 1b, grey dashed trace) [19], and by using a smaller potential window limited to the gold electrochemical double layer (EDL) formation region
Summary
Sickle cell anemia is a common inherited blood disorder that leads to major morbidity and early mortality [1,2,3,4]. We modified the sensing electrodes with a MoS2 monolayer selectively electrodeposited using two different electronic polarization waveforms in order to fine-tune the specific electronic properties of the TMDC material This resulted in the electrochemical differentiation of HU from the main redox active interfering molecules contained in blood, uric (UA), and ascorbic (AA) acids. We have been using chemometric analysis [24,25,35], allowing us to quantify the drug HU with a sensitivity of 37 nM cm−2 μA−1 and a limit of detection (LoD) as low as 22 nM in undiluted human serum This new technique is both novel and innovative, as it offers an opportunity to measure HU with expensive technology and potentially even at the Biomedicines 2021, 9, x FOR PEER REVIEW point-of-care. United States), calcium chloride (97%, 10195054 Alfa Aesar), iron sulfate hydrate (97%, 307718, Sigma-Aldrich), hydrochloric acid (32%, 00846050100, Bio-Lab Ltd.), sulfuric acid
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