Signal promoting role of a <i>p</i>-type transition metal dichalcogenide used for the detection of ultra-trace amounts of diclofenac via a labeled aptasensor

doi:10.1007/s11705-019-1797-0

Front. Chem. Sci. Eng.

2019, Vol. 13

Issue (4) : 823-831 https://doi.org/10.1007/s11705-019-1797-0

RESEARCH ARTICLE

Signal promoting role of a p-type transition metal dichalcogenide used for the detection of ultra-trace amounts of diclofenac via a labeled aptasensor

Abdolhamid Hatefi-Mehrjardi(

), Amirkhosro Beheshti-Marnani(

), Zarrin Es'haghi

Department of Chemistry, Payame Noor University (PNU), Tehran, Iran

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Abstract

A p-type transition metal dichalcogenide (WS₂) was synthesized and hybridized with graphene oxide via a simple hydrothermal method. The as-prepared material was used to modify a glassy carbon electrode for the fabrication of a simple, stable, and repeatable methylene blue-labeled “signal-off” aptasensor used for the sensitive determination of very low amounts of sodium diclofenac (DCF). The synthetic material, modification process, and role of WS₂ in the current response enhancement were studied by X-ray diffraction, energy-dispersive X-ray spectroscopy, field emission scanning electron microscopy, high resolution transmission electron microscopy, Hall effect, cyclic voltammetry, differential pulse voltammetry, and electrochemical impedance spectroscopy. Subsequently, a wide linear range of DCF concentration (0.5–300 nmol/L), very low limit of detection (0.23 nmol/L), and good selectivity were obtained using the differential pulse voltammetry method with the assembled aptasensor. Finally, the fabricated aptasensor was successfully developed for physiological real samples with significant recoveries.

Keywords labeled aptasensor transition metal dichalcogenide graphene oxide sodium diclofenac

Corresponding Author(s): Abdolhamid Hatefi-Mehrjardi,Amirkhosro Beheshti-Marnani

Online First Date: 22 April 2019 Issue Date: 04 December 2019

Cite this article:

Abdolhamid Hatefi-Mehrjardi,Amirkhosro Beheshti-Marnani,Zarrin Es'haghi. Signal promoting role of a p-type transition metal dichalcogenide used for the detection of ultra-trace amounts of diclofenac via a labeled aptasensor[J]. Front. Chem. Sci. Eng., 2019, 13(4): 823-831.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1797-0
https://academic.hep.com.cn/fcse/EN/Y2019/V13/I4/823

Fig.1 (A) XRD pattern and (B) EDX elemental analysis of the as-synthesized WS₂

Fig.2 FESEM images of the as-synthesized (A) GO and (C) WS₂ samples, and (D) the WS₂/GO nanohybrid; (B) HRTEM images of the transparent graphene nanosheets and (E) the synthetic WS₂/GO nanohybrid

Fig.3 (A) Plot of CV current response versus DCF amino-aptamer concentration used to immobilize the aptamer on the surface of the graphene-modified GCE upon incubation in 25 µmol/L of MB⁺; (B) CV curves obtained for the DCF amino-aptamer-modified GCEs (assembled using an initial concentration of aptamer= 2 µmol/L) incubated in 25 µmol/L of MB⁺ with different mass ratios of WS₂:GO (mg:mg): (a) 0:100, (b) 5:95, (c) 7:93, (d) 10:90, (e) 13:87, and (f) 17:83

Fig.4 (A) CV curves recorded for the MB⁺ bonded DCF aptasensor at various scan rates and (B) plot of the linear relationship between the extracted anodic and cathodic peak currents versus scan rate

Fig.5 (A) CV curves and (B) Nyquist plots obtained for the MB⁺-bonded DCF amino-aptamer immobilized on the WS₂:GO (10 mg:90 mg)-modified GCE in the (a) absence and presence of (b) 500 nmol/L and (c) 500 µmol/L DCF. The scan rate for CV was 50 mV/s and the EIS tests were performed in the presence of K₃Fe (CN)₆ (10 mmol/L) at E_dc = 0.230 V and E_ac = 5 mV over a frequency range of 10 kHz–40 MHz. The inset shows the Randles’ equivalent circuit used for fitting the EIS data (R_s = electrolyte resistance, CPE = constant phase element, R_ct = charge transfer resistance, and W = Warburg impedance)

Fig.6 Schematic representation of the DCF aptasensor assembly process, which describes the “signal-off” detection mode of the fabricated biosensor (note that this schematic may not be in the scale of the immobilized aptamer and DCF molecules)

Fig.7 (A) DPV response of the fabricated aptasensor incubated with 25 µmol/L of MB⁺ in: (a) blank PBS (0.1 mol/L, pH 7.2) and (b-g) 0.5?300 nmol/L DCF in the same PBS solution; (B) the corresponding calibration line plot

Fig.8 Interference effects of PA and CZ on the response of the fabricated aptasensor incubated in 25 µmol/L of MB⁺ for 50 nmol/L and 200 nmol/L of DCF, and a mixture of drugs

Tab.1 Recoveries of DCF obtained from human physiological fluids used as real samples

Tab.2 Comparison of the current work with recent investigations on the determination of DCF

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