1. Electrochemical and electronic detection of biomarkers in serum: a systematic comparison using aptamer-functionalized surfaces
- Author
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Henri Happy, Wolfgang Knoll, Patrik Aspermair, Vladyslav Mishyn, Yann R. Leroux, Teresa Rodrigues, Rabah Boukherroub, Laura Butruille, Sabine Szunerits, David Montaigne, Eloise Woitrain, Institut d’Électronique, de Microélectronique et de Nanotechnologie - UMR 8520 (IEMN), Centrale Lille-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Université Polytechnique Hauts-de-France (UPHF)-JUNIA (JUNIA), Université catholique de Lille (UCL)-Université catholique de Lille (UCL), Austrian Institute of Technology [Vienna] (AIT), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Récepteurs Nucléaires, Maladies Métaboliques et Cardiovasculaires (RNMCD - U1011), Institut Pasteur de Lille, Réseau International des Instituts Pasteur (RIIP)-Réseau International des Instituts Pasteur (RIIP)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Université de Lille-Centre Hospitalier Régional Universitaire [Lille] (CHRU Lille), Carbon - IEMN (CARBON - IEMN), Université catholique de Lille (UCL)-Université catholique de Lille (UCL)-Centrale Lille-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Université Polytechnique Hauts-de-France (UPHF)-JUNIA (JUNIA), Danube Private University [Krems, Autriche] (DPU), NanoBioInterfaces - IEMN (NBI - IEMN), Financial support from the Centre National de la Recherche Scientifique (CNRS), the University of Lille, the Hauts-de-France region and the CPER 'Photonics for Society' is gratefully acknowledged. Financial support came further from the FFG, Austria, within the Comet program., IEMN, Collection, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), and Récepteurs Nucléaires, Maladies Métaboliques et Cardiovasculaires - U1011 (RNMCD)
- Subjects
Analyte ,Aptamer ,[SPI] Engineering Sciences [physics] ,02 engineering and technology ,Biosensing Techniques ,010402 general chemistry ,01 natural sciences ,Biochemistry ,Graphene-based field-effect transistor ,Analytical Chemistry ,[SPI]Engineering Sciences [physics] ,Limit of Detection ,Troponin I ,Humans ,Detection limit ,Chromatography ,Chemistry ,Differential pulse voltammetry ,Electrochemical Techniques ,Aptamers, Nucleotide ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Electrochemical gas sensor ,Dissociation constant ,Ionic strength ,cTnI ,0210 nano-technology ,Biomarkers - Abstract
International audience; Sensitive and selective detection of biomarkers in serum in a short time has a significant impact on health. The enormous clinical importance of developing reliable methods and devices for testing serum levels of cardiac troponin I (cTnI), which are directly correlated to acute myocardial infarction (AMI), has spurred an unmatched race among researchers for the development of highly sensitive and cost-effective sensing formats to be able to differentiate patients with early onset of cardiac injury from healthy individuals with a mean cTnI level of 26 pg mL-1. Electronic- and electrochemical-based detection schemes allow for fast and quantitative detection not otherwise possible at the point of care. Such approaches rely largely on voltammetric and field-effect-based readouts. Here, we systematically investigate electric and electrochemical point-of-care sensors for the detection of cTnI in serum samples by using the same surface receptors, cTnI aptamer-functionalized CVD graphene-coated interdigated gold electrodes. The analytical performances of both sensors are comparable with a limit of detection (LoD) of 5.7 ± 0.6 pg mL-1(electrochemical) and 3.3 ± 1.2 pg mL-1 (electric). However, both sensors exhibit different equilibrium dissociation constant (KD) values between the aptamer-linked surface receptor and the cTnI analyte, being 160 pg mL-1 for the electrochemical and about three times lower for the electrical approach with KD = 51.4 pg mL-1. This difference is believed to be related to the use of a redox mediator in the electrochemical sensor for readout. The ability of the redox mediator to diffuse from the solution to the surface via the cTnI/aptamer interface is hindered, correlating to higher KD values. In contrast, the electric readout has the advantage of being label-free with a sensing limitation due to ionic strength effects, which can be limited using poly(ethylene) glycol surface ligands.
- Published
- 2022
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