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Biofunctionalization of Graphene-Based FET Sensors through Heterobifunctional Nanoscaffolds: Technology Validation toward Rapid COVID-19 Diagnostics and Monitoring

Publication year: 2022
Authors: Piccinini E. *, Fenoy G.E. , Cantillo A.L. , Allegretto J.A. , Scotto J. , Piccinini J.M. , Marmisollé W.A. , Azzaroni O. *
Affiliations:

Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas (INIFTA), Departamento de Química, Facultad de Ciencias Exactas, Universidad Nacional de La Plata (UNLP), CONICET. 64 and 113, Buenos Aires 1900, Argentina

Published in: Advanced Materials Interfaces, 2102526
doi: https://doi.org/10.1002/admi.202102526

The biofunctionalization of graphene field-effect transistors (GFETs) through vinylsulfonated-polyethyleneimine nanoscaffold is presented for enhanced biosensing of severe acute respiratory-related coronavirus 2 (SARS-CoV-2) spike protein and human ferritin, two targets of great importance for the rapid diagnostic and monitoring of individuals with COVID-19. The heterobifunctional nanoscaffold enables covalent immobilization of binding proteins and antifouling polymers while the whole architecture is attached to graphene by multivalent π–π interactions. First, to optimize the sensing platform, concanavalin A is employed for glycoprotein detection. Then, monoclonal antibodies specific against SARS-CoV-2 spike protein and human ferritin are anchored, yielding biosensors with limit of
detections of 0.74 and 0.23 nm, and apparent affinity constants (K GFET D ) of 6.7 and 8.8 nm, respectively. Both biosensing platforms show good specificity, fast time response, and wide dynamic range (0.1–100 nm). Moreover, SARS-CoV-2 spike protein is also detected in spiked nasopharyngeal swab
samples. To rigorously validate this biosensing technology, the GFET response is matched with surface plasmon resonance measurements, exhibiting linear correlations (from 2 to 100 ng cm−2) and good agreement in terms of KD values. Finally, the performance of the biosensors fabricated through the nanoscaffold strategy is compared with those obtained through the widely employed monopyrene approach, showing enhanced sensitivity.