J Am Chem Soc. 2025 Apr 3. doi: 10.1021/jacs.5c03552. Online ahead of print.
ABSTRACT
Diabetes mellitus, a prevalent metabolic disorder affecting hundreds of millions of people worldwide, demands continuous glucose monitoring for effective management. Current blood glucose monitoring methods, such as commercial glucometers, are accurate but are often perceived as uncomfortable. Motivated by the need for noninvasive, ultrasensitive alternatives, our study presents electrolyte-gated graphene field-effect transistors functionalized with glucose oxidase. We developed an optimized fabrication process that integrates a 32-transistor matrix within a miniaturized 1000 μm2 footprint, ensuring high device uniformity while enabling detection in 40 μL analyte volume. A comprehensive suite of techniques─including Raman spectroscopy, X-ray photoelectron spectroscopy, and water contact angle measurements─reveals the stepwise evolution of graphene chemistry and surface properties leading to the controlled immobilization of glucose oxidase. Our findings demonstrate p-type doping and tensile strain in the graphene channel across the nanomolar-millimolar glucose concentration range. The enzyme-catalyzed oxidation of glucose produces hydrogen peroxide in close proximity to the graphene channel, inducing a systematic shift in the Dirac point voltage toward more positive values. Under these conditions, the biosensor achieves an attomolar limit of detection and a sensitivity of 10.6 mV/decade, outperforming previously reported glucose sensors. Selectivity tests against common interferents such as lactate and ascorbic acid, as well as validation in artificial and human tears, demonstrate its robustness for real-world applications. Altogether, these findings position the electrolyte-gated graphene field-effect transistor as a transformative, noninvasive glucose-sensing platform, paving the way for next-generation continuous monitoring devices, including wearable formats for real-time, user-friendly diabetes management.
PMID:40179421 | DOI:10.1021/jacs.5c03552