4.6 Article

Enhanced Photoelectrochemical Detection of an Analyte Triggered by Its Concentration by a Singlet Oxygen-Generating Fluoro Photosensitizer

Journal

ACS SENSORS
Volume 5, Issue 11, Pages 3501-3509

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acssensors.0c01609

Keywords

singlet oxygen; rifampicin; antibiotic; photocatalysis; phthalocyanine

Funding

  1. ERA.Net RUS Plus Plasmon Electrolight project (Belgium) [18-53-76006 ERA]
  2. BOF-UAntwerp funding
  3. Center for Functional Materials, Seton Hall University (USA)
  4. European Social Fund, Human Capital Operational Programme 2014-2020 [POCU/380/6/13/125171]

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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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