Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes

The use of enzyme-based biosensors for the detection and quantification of analytes of interest such as contaminants of emerging concern, including over-the-counter medication, provides an attractive alternative compared to more established techniques. However, their direct application to real envir...

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Main Authors: Marcela Herrera-Domínguez, Koun Lim, Iris Aguilar-Hernández, Alejandra García-García, Shelley D. Minteer, Nancy Ornelas-Soto, Raúl Garcia-Morales
Format: Article
Language:English
Published: MDPI AG 2023-05-01
Series:Sensors
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Online Access:https://www.mdpi.com/1424-8220/23/10/4633
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author Marcela Herrera-Domínguez
Koun Lim
Iris Aguilar-Hernández
Alejandra García-García
Shelley D. Minteer
Nancy Ornelas-Soto
Raúl Garcia-Morales
author_facet Marcela Herrera-Domínguez
Koun Lim
Iris Aguilar-Hernández
Alejandra García-García
Shelley D. Minteer
Nancy Ornelas-Soto
Raúl Garcia-Morales
author_sort Marcela Herrera-Domínguez
collection DOAJ
description The use of enzyme-based biosensors for the detection and quantification of analytes of interest such as contaminants of emerging concern, including over-the-counter medication, provides an attractive alternative compared to more established techniques. However, their direct application to real environmental matrices is still under investigation due to the various drawbacks in their implementation. Here, we report the development of bioelectrodes using laccase enzymes immobilized onto carbon paper electrodes modified with nanostructured molybdenum disulfide (MoS<sub>2</sub>). The laccase enzymes were two isoforms (LacI and LacII) produced and purified from the fungus <i>Pycnoporus sanguineus</i> CS43 that is native to Mexico. A commercial purified enzyme from the fungus <i>Trametes versicolor</i> (TvL) was also evaluated to compare their performance. The developed bioelectrodes were used in the biosensing of acetaminophen, a drug widely used to relieve fever and pain, and of which there is recent concern about its effect on the environment after its final disposal. The use of MoS<sub>2</sub> as a transducer modifier was evaluated, and it was found that the best detection was achieved using a concentration of 1 mg/mL. Moreover, it was found that the laccase with the best biosensing efficiency was LacII, which achieved an LOD of 0.2 µM and a sensitivity of 0.108 µA/µM cm<sup>2</sup> in the buffer matrix. Moreover, the performance of the bioelectrodes in a composite groundwater sample from Northeast Mexico was analyzed, achieving an LOD of 0.5 µM and a sensitivity of 0.015 µA/µM cm<sup>2</sup>. The LOD values found are among the lowest reported for biosensors based on the use of oxidoreductase enzymes, while the sensitivity is the highest currently reported.
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spelling doaj.art-4b46a244caa64bde8e4238b7530247a02023-11-18T03:10:13ZengMDPI AGSensors1424-82202023-05-012310463310.3390/s23104633Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper ElectrodesMarcela Herrera-Domínguez0Koun Lim1Iris Aguilar-Hernández2Alejandra García-García3Shelley D. Minteer4Nancy Ornelas-Soto5Raúl Garcia-Morales6Laboratorio de Nanotecnología Ambiental, Escuela de Ingeniería y Ciencias, Tecnológico de Monterrey, Ave. Eugenio Garza Sada 2501, Monterrey 64849, NL, MexicoDepartment of Chemistry and Materials Science & Engineering, University of Utah, Salt Lake City, UT 84112, USALaboratorio de Nanotecnología Ambiental, Escuela de Ingeniería y Ciencias, Tecnológico de Monterrey, Ave. Eugenio Garza Sada 2501, Monterrey 64849, NL, MexicoLaboratorio de Síntesis y Modificación de Nanoestructuras y Materiales Bidimensionales, Centro de Investigación en Materiales Avanzados S.C., Unidad Monterrey, Parque PIIT, Apodaca 66628, NL, MexicoDepartment of Chemistry and Materials Science & Engineering, University of Utah, Salt Lake City, UT 84112, USALaboratorio de Nanotecnología Ambiental, Escuela de Ingeniería y Ciencias, Tecnológico de Monterrey, Ave. Eugenio Garza Sada 2501, Monterrey 64849, NL, MexicoCentro de Nanociencias y Nanotecnología, Universidad Nacional Autónoma de México, Carretera Tijuana-Ensenada Km. 107, Ensenada 22860, BC, MexicoThe use of enzyme-based biosensors for the detection and quantification of analytes of interest such as contaminants of emerging concern, including over-the-counter medication, provides an attractive alternative compared to more established techniques. However, their direct application to real environmental matrices is still under investigation due to the various drawbacks in their implementation. Here, we report the development of bioelectrodes using laccase enzymes immobilized onto carbon paper electrodes modified with nanostructured molybdenum disulfide (MoS<sub>2</sub>). The laccase enzymes were two isoforms (LacI and LacII) produced and purified from the fungus <i>Pycnoporus sanguineus</i> CS43 that is native to Mexico. A commercial purified enzyme from the fungus <i>Trametes versicolor</i> (TvL) was also evaluated to compare their performance. The developed bioelectrodes were used in the biosensing of acetaminophen, a drug widely used to relieve fever and pain, and of which there is recent concern about its effect on the environment after its final disposal. The use of MoS<sub>2</sub> as a transducer modifier was evaluated, and it was found that the best detection was achieved using a concentration of 1 mg/mL. Moreover, it was found that the laccase with the best biosensing efficiency was LacII, which achieved an LOD of 0.2 µM and a sensitivity of 0.108 µA/µM cm<sup>2</sup> in the buffer matrix. Moreover, the performance of the bioelectrodes in a composite groundwater sample from Northeast Mexico was analyzed, achieving an LOD of 0.5 µM and a sensitivity of 0.015 µA/µM cm<sup>2</sup>. The LOD values found are among the lowest reported for biosensors based on the use of oxidoreductase enzymes, while the sensitivity is the highest currently reported.https://www.mdpi.com/1424-8220/23/10/4633electrochemical biosensoracetaminophenlaccasesMoS<sub>2</sub>emerging pollutants
spellingShingle Marcela Herrera-Domínguez
Koun Lim
Iris Aguilar-Hernández
Alejandra García-García
Shelley D. Minteer
Nancy Ornelas-Soto
Raúl Garcia-Morales
Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes
Sensors
electrochemical biosensor
acetaminophen
laccases
MoS<sub>2</sub>
emerging pollutants
title Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes
title_full Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes
title_fullStr Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes
title_full_unstemmed Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes
title_short Detection of Acetaminophen in Groundwater by Laccase-Based Amperometric Biosensors Using MoS<sub>2</sub> Modified Carbon Paper Electrodes
title_sort detection of acetaminophen in groundwater by laccase based amperometric biosensors using mos sub 2 sub modified carbon paper electrodes
topic electrochemical biosensor
acetaminophen
laccases
MoS<sub>2</sub>
emerging pollutants
url https://www.mdpi.com/1424-8220/23/10/4633
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