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Harnessing Small-Molecule Analyte Detection in Complex Media: Combining Molecularly Imprinted Polymers, Electrolytic Transistors, and Machine Learning
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    Harnessing Small-Molecule Analyte Detection in Complex Media: Combining Molecularly Imprinted Polymers, Electrolytic Transistors, and Machine Learning
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    • Gabrielle Coelho Lelis
      Gabrielle Coelho Lelis
      Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, SP 13083-100, Brazil
    • Wilson Tiago Fonseca
      Wilson Tiago Fonseca
      Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, SP 13083-100, Brazil
    • Alessandro Henrique de Lima
      Alessandro Henrique de Lima
      Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, SP 13083-100, Brazil
    • Anderson Kenji Okazaki
      Anderson Kenji Okazaki
      Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, SP 13083-100, Brazil
    • Eduardo Costa Figueiredo
      Eduardo Costa Figueiredo
      Faculty of Pharmaceutical Sciences, Federal University of Alfenas, Alfenas, MG 37130-001, Brazil
    • Antonio Riul Jr
      Antonio Riul Jr
      Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin, Campinas, SP 13083-859, Brazil
    • Gabriel Ravanhani Schleder
      Gabriel Ravanhani Schleder
      Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, SP 13083-100, Brazil
      John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, United States
    • Paolo Samorì
      Paolo Samorì
      Université de Strasbourg, CNRS, ISIS, 8 allée Gaspard Monge, Strasbourg 67000, France
    • Rafael Furlan de Oliveira*
      Rafael Furlan de Oliveira
      Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, SP 13083-100, Brazil
      Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin, Campinas, SP 13083-859, Brazil
      *[email protected]
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, XXXX, XXX, XXX-XXX
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    https://doi.org/10.1021/acsami.3c16699
    Published December 22, 2023
    © 2023 American Chemical Society

    Abstract

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    Small-molecule analyte detection is key for improving quality of life, particularly in health monitoring through the early detection of diseases. However, detecting specific markers in complex multicomponent media using devices compatible with point-of-care (PoC) technologies is still a major challenge. Here, we introduce a novel approach that combines molecularly imprinted polymers (MIPs), electrolyte-gated transistors (EGTs) based on 2D materials, and machine learning (ML) to detect hippuric acid (HA) in artificial urine, being a critical marker for toluene intoxication, parasitic infections, and kidney and bowel inflammation. Reduced graphene oxide (rGO) was used as the sensory material and molecularly imprinted polymer (MIP) as supramolecular receptors. Employing supervised ML techniques based on symbolic regression and compressive sensing enabled us to comprehensively analyze the EGT transfer curves, eliminating the need for arbitrary signal selection and allowing a multivariate analysis during HA detection. The resulting device displayed simultaneously low operating voltages (<0.5 V), rapid response times (≤10 s), operation across a wide range of HA concentrations (from 0.05 to 200 nmol L–1), and a low limit of detection (LoD) of 39 pmol L–1. Thanks to the ML multivariate analysis, we achieved a 2.5-fold increase in the device sensitivity (1.007 μA/nmol L–1) with respect to the human data analysis (0.388 μA/nmol L–1). Our method represents a major advance in PoC technologies, by enabling the accurate determination of small-molecule markers in complex media via the combination of ML analysis, supramolecular analyte recognition, and electrolytic transistors.

    © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.3c16699.

    • Device fabrication steps, XPS and Raman characterization of GO and rGO films, rGO EGT operational characteristics and stability, XPS analysis of the device gate electrode after modification with MIP, and multivariate machine learning analysis (PDF)

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    This article is cited by 3 publications.

    1. Guilherme Segolin Selmi, Eduardo Rodrigues Lourenço Neto, Gabrielle Coelho Lelis, Anderson Kenji Okazaki, Antonio Riul, Maria Luisa Braunger, Rafael Furlan de Oliveira. Pulse Dynamics in Reduced Graphene Oxide Electrolyte‐Gated Transistors: Charge Memory Effects and Mechanisms Governing the Ion‐To‐Electron Transduction. Advanced Electronic Materials 2024, https://doi.org/10.1002/aelm.202400791
    2. Lei Fan, Zhaobing Su, Xiyang Liu, Yuping Wang. Decomposition based cross-parallel multiobjective genetic programming for symbolic regression. Applied Soft Computing 2024, 167 , 112239. https://doi.org/10.1016/j.asoc.2024.112239
    3. Yanmei Sun, Yufei Wang, Qi Yuan. Artificial nociceptor based on temperature responsive of synaptic transistor for electronic skin. Applied Materials Today 2024, 40 , 102355. https://doi.org/10.1016/j.apmt.2024.102355

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, XXXX, XXX, XXX-XXX
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.3c16699
    Published December 22, 2023
    © 2023 American Chemical Society

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