Advanced Electrochemical Sensors for the Determination of Selected Antibiotic Drug Residues in Food and Water Samples
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Date
2024-06
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Addis Ababa University
Abstract
The presence of antibiotic drug residues in food and water sources poses a critical challenge to the public health and environmental sustainability. Addressing this challenge requires the development of highly sensitive and selective detection methods capable of accurately quantifying trace levels of the residues in complex sample matrices. The aim of this study was to contribute to this vital area of research by focusing on the designing, fabrication, characterization, and application of advanced electrochemical sensors for the detection of antibiotic residues in various matrices. In this study, eight cutting-edge electrochemical sensors were developed, characterized, and successfully applied for the individual and simultaneous determination of selected antibiotic drug residues in food and water samples. Through thorough experimentation and optimization, novel electrochemical sensor architectures have been developed using innovative materials, including gold-silver alloy nanocoral clusters (Au-Ag-ANCCs), thermally annealed gold–silver alloy nanoporous matrices (TA-Au-Ag-ANpM), iron-doped polyaniline (Fe-dop-PANI), nickel oxide nanoparticles (NiO-NPs), zinc oxide nanoparticles (ZnO-NPs), functionalized multi-walled carbon nanotubes (f-MWCNTs), reduced graphene oxide (r-GO), poly(L-histidine), poly(L-serine), poly(glycine), polyethylene oxide (PEO), and choline chloride (ChCl), to improve sensitivity, selectivity, and stability. The surface morphology, elemental composition, and electrochemical properties of the developed sensors were characterized using an array of analytical techniques, including UV–Vis spectroscopy, Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction spectroscopy (XRD), energy dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS), and cyclic voltammetry (CV). Among the developed sensors, ChCl/CPE was designed for the determination of ciprofloxacin (CPRO) in eye drops, river water, and egg samples. It exhibited outstanding performance with a wide linear range (0.005–200 μM), and impressive detection and quantification limits of 0.36 nM and 1.2 nM, respectively. ChCl/GCE was prepared for the simultaneous determination of tinidazole (TIN) and chloramphenicol (CAP) in egg, honey, and milk samples. It showed exceptional detection capability with a wide linear range of 0.010–170 μM and 0.005–300 μM for TIN and CAP, respectively. The limit of detection (LOD) and limit of quantification (LOQ) were 0.90 nM and 3.0 nM for TIN, and 0.27 nM and 0.89 nM for CAP, respectively. TA-Au-Ag-ANpM/r-GO/poly(glycine)/GCE was developed for the detection of life-threatening residues of metronidazole (MTZ) in milk powder, pork, and chicken meat samples. It
performed exceptionally in the detection of MTZ with a wide linear range from 2.0 pM to 410 μM. The LOD and LOQ were determined to be 0.0312 pM and 0.104 pM, respectively. Au-Ag-ANCCs/r-GO/poly(L-histidine)/GCE was used for the simultaneous determination of vancomycin (VAN) and ceftriaxone (CFT) residues in chicken meat, fish, and milk samples. The sensor demonstrated outstanding performance in the determination of the analytes over a wide dynamic range, from 1.0 pM to 120 μM for VAN and from 1.0 pM to 290 μM for CFT. The LOD and LOQ values were determined to be 0.11 pM and 0.36 pM for VAN and 0.017 pM and 0.057 pM for CFT, respectively. TA-Au-Ag-ANpM/f-MWCNTs-CPE/poly(L-serine) was prepared for the simultaneous detection of sulfathiazole (SFT) and sulfamethoxazole (SFM) residues in honey, beef, and egg samples. It showed exceptional performance in a wide linear range (4.0 pM to 490 μM for SFT and 4.0 pM to 520 μM for SFM), with picomolar detection and quantification limits (0.53 pM and 1.75 pM for SFT, 0.41 pM and 1.35 pM for SFM). Au-Ag-ANCCs/f-MWCNTs-CPE/ChCl was developed for the simultaneous determination of rifampicin (RAMP) and norfloxacin (NFX) residues in water samples. It exhibited outstanding performance in a broad linear range, from 14 pM to 115 μM for RAMP and from 0.9 nM to 200 μM for NFX, with LOD and LOQ values of 2.7 pM and 8.85 pM for RAMP and 0.14 nM and 0.47 nM for NFX, respectively. Au-Ag-ANCCs/ZnO-NPs-CPE/PEO was prepared for the simultaneous detection of nitrofurantoin (NFT) and furazolidone (FZD) in poultry, fish, honey, dairy products, and municipal wastewater samples. The sensor demonstrated exceptional performance over a wide linear range, from 1.0 pM to 250 μM for NFT and 0.9 nM to 360 μM for FZD. The LOD and LOQ were found to be 0.26 pM and 0.88 pM for NFT and 0.023 pM and 0.076 pM for FZD, respectively. Finally, TA-Au-Ag-ANpM/Fe-dop-PANI/NiONPs/GCE was developed for simultaneously determining azithromycin (AZM) and enrofloxacin (ENF) residues in food and water samples. The sensor exhibited exceptional performance in a broad dynamic range from 0.8 pM to 250 μM for AZM and 0.1 pM to 550 μM for ENF, with LOD and LOQ values of 0.053 pM and 0.18 pM for AZM and 0.013 pM and 0.042 pM for ENF, respectively. In order to maximize the efficiency of the proposed sensors, an extensive optimization of various experimental parameters was performed. The optimization process included the selection of the appropriate supporting electrolytes, choice of the pH of the electrolyte solutions, determination of the number of electropolymerization cycles, optimization of the mixing ratio of the nanocomposites, adjustment of the volume of the drop-casting species, and selection of the square wave voltammetry (SWV) parameters, such as amplitude, frequency, and step potential, as
well as other instrumental parameters. Under these optimized experimental conditions, the developed sensors exhibited remarkable selectivity and effectively discriminated between the target analytes and interferents present in complex sample matrices. In addition, the developed sensors exhibited exceptional reproducibility, repeatability, and long-term stability. Subsequently, the developed sensors were validated using real food and water samples that were suspected to contain antimicrobial drug residues. The results revealed impressive recoveries ranging from 95.6 to 103%, with relative standard deviations below 5%. In general, the results presented in this paper represent a significant advance in the field of electrochemical sensor technology, particularly in the vital area of identifying antibiotic residues in food and water samples. The introduction of these state-of-the-art sensors heralds a new era characterized by increased sensitivity, selectivity, and reliability. This advancement will change the landscape of monitoring, regulating, and controlling antibiotic residues in food chains and water sources. Beyond enriching scientific knowledge, this breakthrough offers tangible benefits for public health and environmental sustainability, and embodies the laudable pursuit of advancing knowledge for the benefit of society.
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Keywords
Antibiotic Resides, Electrochemical Sensors, Nanocomposite Modifiers, Food Samples, Water Samples