Harnessing Small-Molecule Analyte Detection in Complex Media: Combining Molecularly Imprinted Polymers, Electrolytic Transistors, and Machine Learning

Author(s)

Lelis, Gabrielle Coelho ; Fonseca, Wilson Tiago ; de Lima, Alessandro Henrique ; Okazaki, Anderson Kenji ; Figueiredo, Eduardo Costa ; Riul Jr, Antonio ; Schleder, Gabriel Ravanhani ; Samori, Paolo ; de Oliveira, Rafael Furlan

• Document type: Journal article
• Source: ACS APPLIED MATERIALS & INTERFACES; v. N/A, p. 11-pg., 2023-12-22.

Abstract

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 mu A/nmol L-1) with respect to the human data analysis (0.388 mu A/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. (AU)

• FAPESP's process: 23/03501-2 - Evaluation of the Operational Characteristics and Stability of Liquid-gated Transistors based on Reduced Graphene Oxide in Artificial Fluids for Biosensing Applications
• Grantee: Gabrielle Coelho Lelis
• Support Opportunities: Scholarships in Brazil - Scientific Initiation
• FAPESP's process: 21/06238-5 - Functionalized solution-processed 2D materials: development of prototyping electric sensors and biosensors
• Grantee: Rafael Furlan de Oliveira
• Support Opportunities: Research Grants - Young Investigators Grants
• FAPESP's process: 19/14949-9 - EMU: multiuser infrastructure dedicated to nanofabrication and characterization of nanodevices at LNNano/CNPEM
• Grantee: Edson Roberto Leite
• Support Opportunities: Multi-user Equipment Program