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Author |
Blidar, A.-M. |
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Title |
The development of sensitive and selective electrochemical methods for the detection of antibiotics |
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Doctoral thesis |
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Year  |
2021 |
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139 p. |
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Doctoral thesis; Pharmacology. Therapy; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab) |
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Abstract |
The discovery of antibiotics represented one of the greatest breakthroughs in medicine. Their success combined with an increasing intensive use is apparently bound to be also their undoing. This is due to the development of acquired antibiotic resistance, leading to inefficient antibiotherapy and even to the impossibility of treatment and death. The development and spread of antibiotic resistance are fueled by the widespread presence of trace levels of antibiotics residue, in various media, from environment to aliments. One of the solutions is the rigorous monitoring of the levels of antibiotics, which in term requires an almost constant development of new, more accessible analytical methods, especially screening methods, capable of decentralized analysis. In this direction, the electrochemical detection of antibiotics represents a very viable alternative. In this context, the aim of this thesis was to develop new electrochemical methods for the detection of antibiotics by employing and expanding on several strategies, like biomimetic sensors and electrochemical fingerprinting. Five studies were described in this thesis, that can be roughly divided in three categories, based on the analytical strategy employed. The first group is represented by direct electrochemical methods. The second group focuses on the use of biomimetic elements, molecularly imprinted polymers and aptamers. The hyphenation of electrochemical methods with other analytical methods was explored in the last group. In the last study, included in this group, the singlet oxygen-based photoelectrochemical approach was used for the detection of a phenolic antibiotic, rifampicin. The originality of the thesis consists in the testing and development of new approaches to various strategies used in electrochemical detection, revealing new insights in the field of electrochemical detection of antibiotics. The complex electrochemical fingerprint and the mechanism of the electrochemical oxidation were created and investigated, respectively, for the antibiotic vancomycin. New sensitive nanoplatforms were prepared by employing and combining new protocols. Additionally, important contributions were brought through the study involving the singlet oxygen-based detection of rifampicin. We demonstrated how a photocatalyst can exhibit analyte selectivity by strongly interacting with a complex phenolic compound, rifampicin. Summing up, the studies presented in this thesis will have an important impact in the field of electrochemical detection of antibiotics. |
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Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:182955 |
Serial |
7804 |
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Author |
Blidar, A.; Trashin, S.; Carrion, E.N.; Gorun, S.M.; Cristea, C.; De Wael, K. |
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Title |
Enhanced photoelectrochemical detection of an analyte triggered by its concentration by a singlet oxygen-generating fluoro photosensitizer |
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A1 Journal article |
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Year |
2020 |
Publication |
Acs Sensors |
Abbreviated Journal |
Acs Sensors |
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Volume |
5 |
Issue |
11 |
Pages |
3501-3509 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation) |
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Abstract |
The use of a photocatalyst (photosensitizer) which produces singlet oxygen instead of enzymes for oxidizing analytes creates opportunities for designing cost-efficient and sensitive photoelectrochemical sensors. We report that perfluoroisopropyl-substituted zinc phthalocyanine (F64PcZn) interacts specifically with a complex phenolic compound, the antibiotic rifampicin (RIF), but not with hydroquinone or another complex phenolic compound, the antibiotic doxycycline. The specificity is imparted by the selective preconcentration of RIF in the photocatalytic layer, as revealed by electrochemical and optical measurements, complemented by molecular modeling that confirms the important role of a hydrophobic cavity formed by the iso-perfluoropropyl groups of the photocatalyst. The preconcentration effect favorably enhances the RIF photoelectrochemical detection limit as well as sensitivity to nanomolar (ppb) concentrations, LOD = 7 nM (6 ppb) and 2.8 A.M-1.cm(-2), respectively. The selectivity to RIF, retained in the photosensitizer layer, is further enhanced by the selective removal of all unretained phenols via simple washing of the electrodes with pure buffer. The utility of the sensor for analyzing municipal wastewater was demonstrated. This first demonstration of enhanced selectivity and sensitivity due to intrinsic interactions of a molecular photocatalyst (photosensitizer) with an analyte, without use of a biorecognition element, may allow the design of related, robust, simple, and viable sensors. |
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000595550100021 |
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2020-10-29 |
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2379-3694 |
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UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.9 |
Times cited |
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Open Access |
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Most recent IF: 8.9; 2020 IF: NA |
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Call Number |
UA @ admin @ c:irua:176057 |
Serial |
7913 |
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