Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat

Tetracycline (TC) is a widely known antibiotic used worldwide to treat animals. Its residues in animal-origin foods cause adverse health effects to consumers. Low-cost and real-time measuring systems of TC in food samples are, therefore, extremely needed. In this work, a three-electrode sensitive an...

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Main Authors: Biresaw D. Abera, Inmaculada Ortiz-Gómez, Bajramshahe Shkodra, Francisco J. Romero, Giuseppe Cantarella, Luisa Petti, Alfonso Salinas-Castillo, Paolo Lugli, Almudena Rivadeneyra
Format: Article
Language:English
Published: MDPI AG 2021-12-01
Series:Sensors
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Online Access:https://www.mdpi.com/1424-8220/22/1/269
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author Biresaw D. Abera
Inmaculada Ortiz-Gómez
Bajramshahe Shkodra
Francisco J. Romero
Giuseppe Cantarella
Luisa Petti
Alfonso Salinas-Castillo
Paolo Lugli
Almudena Rivadeneyra
author_facet Biresaw D. Abera
Inmaculada Ortiz-Gómez
Bajramshahe Shkodra
Francisco J. Romero
Giuseppe Cantarella
Luisa Petti
Alfonso Salinas-Castillo
Paolo Lugli
Almudena Rivadeneyra
author_sort Biresaw D. Abera
collection DOAJ
description Tetracycline (TC) is a widely known antibiotic used worldwide to treat animals. Its residues in animal-origin foods cause adverse health effects to consumers. Low-cost and real-time measuring systems of TC in food samples are, therefore, extremely needed. In this work, a three-electrode sensitive and label-free sensor was developed to detect TC residues from milk and meat extract samples, using CO<sub>2</sub> laser-induced graphene (LIG) electrodes modified with gold nanoparticles (AuNPs) and a molecularly imprinted polymer (MIP) used as a synthetic biorecognition element. LIG was patterned on a polyimide (PI) substrate, reaching a minimum sheet resistance (R<sub>sh</sub>) of 17.27 ± 1.04 Ω/sq. The <i>o</i>-phenylenediamine (oPD) monomer and TC template were electropolymerized on the surface of the LIG working electrode to form the MIP. Surface morphology and electrochemical techniques were used to characterize the formation of LIG and to confirm each modification step. The sensitivity of the sensor was evaluated by differential pulse voltammetry (DPV), leading to a limit of detection (LOD) of 0.32 nM, 0.85 nM, and 0.80 nM in buffer, milk, and meat extract samples, respectively, with a working range of 5 nM to 500 nM and a linear response range between 10 nM to 300 nM. The sensor showed good LOD (0.32 nM), reproducibility, and stability, and it can be used as an alternative system to detect TC from animal-origin food products.
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spelling doaj.art-7e5e8a3af9bd47e2962efb4e8a555eb02023-11-23T12:19:39ZengMDPI AGSensors1424-82202021-12-0122126910.3390/s22010269Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and MeatBiresaw D. Abera0Inmaculada Ortiz-Gómez1Bajramshahe Shkodra2Francisco J. Romero3Giuseppe Cantarella4Luisa Petti5Alfonso Salinas-Castillo6Paolo Lugli7Almudena Rivadeneyra8Faculty of Science and Technology, Free University of Bolzano, 39100 Bolzano, ItalyDepartment of Analytical Chemistry, University of Granada, 18071 Granada, SpainFaculty of Science and Technology, Free University of Bolzano, 39100 Bolzano, ItalyPervasive Electronics Advanced Research Laboratory (PEARL), Department of Electronics and Computer Technology, University of Granada, 18071 Granada, SpainFaculty of Science and Technology, Free University of Bolzano, 39100 Bolzano, ItalyFaculty of Science and Technology, Free University of Bolzano, 39100 Bolzano, ItalyDepartment of Analytical Chemistry, University of Granada, 18071 Granada, SpainFaculty of Science and Technology, Free University of Bolzano, 39100 Bolzano, ItalyPervasive Electronics Advanced Research Laboratory (PEARL), Department of Electronics and Computer Technology, University of Granada, 18071 Granada, SpainTetracycline (TC) is a widely known antibiotic used worldwide to treat animals. Its residues in animal-origin foods cause adverse health effects to consumers. Low-cost and real-time measuring systems of TC in food samples are, therefore, extremely needed. In this work, a three-electrode sensitive and label-free sensor was developed to detect TC residues from milk and meat extract samples, using CO<sub>2</sub> laser-induced graphene (LIG) electrodes modified with gold nanoparticles (AuNPs) and a molecularly imprinted polymer (MIP) used as a synthetic biorecognition element. LIG was patterned on a polyimide (PI) substrate, reaching a minimum sheet resistance (R<sub>sh</sub>) of 17.27 ± 1.04 Ω/sq. The <i>o</i>-phenylenediamine (oPD) monomer and TC template were electropolymerized on the surface of the LIG working electrode to form the MIP. Surface morphology and electrochemical techniques were used to characterize the formation of LIG and to confirm each modification step. The sensitivity of the sensor was evaluated by differential pulse voltammetry (DPV), leading to a limit of detection (LOD) of 0.32 nM, 0.85 nM, and 0.80 nM in buffer, milk, and meat extract samples, respectively, with a working range of 5 nM to 500 nM and a linear response range between 10 nM to 300 nM. The sensor showed good LOD (0.32 nM), reproducibility, and stability, and it can be used as an alternative system to detect TC from animal-origin food products.https://www.mdpi.com/1424-8220/22/1/269laser-induced grapheneantibiotic residuetetracyclinemolecularly imprinted polymermilkmeat
spellingShingle Biresaw D. Abera
Inmaculada Ortiz-Gómez
Bajramshahe Shkodra
Francisco J. Romero
Giuseppe Cantarella
Luisa Petti
Alfonso Salinas-Castillo
Paolo Lugli
Almudena Rivadeneyra
Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat
Sensors
laser-induced graphene
antibiotic residue
tetracycline
molecularly imprinted polymer
milk
meat
title Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat
title_full Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat
title_fullStr Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat
title_full_unstemmed Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat
title_short Laser-Induced Graphene Electrodes Modified with a Molecularly Imprinted Polymer for Detection of Tetracycline in Milk and Meat
title_sort laser induced graphene electrodes modified with a molecularly imprinted polymer for detection of tetracycline in milk and meat
topic laser-induced graphene
antibiotic residue
tetracycline
molecularly imprinted polymer
milk
meat
url https://www.mdpi.com/1424-8220/22/1/269
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