All-Fiber Flexible Electrochemical Sensor for Wearable Glucose Monitoring.

Abstract

Wearable sensors, specifically microneedle sensors based on electrochemical methods, have expanded extensively with recent technological advances. Today's wearable electrochemical sensors present specific challenges: they show significant modulus disparities with skin tissue, implying possible discomfort in vivo, especially over extended wear periods or on sensitive skin areas. The sensors, primarily based on polyethylene terephthalate (PET) or polyimide (PI) substrates, might also cause pressure or unease during insertion due to the skin's irregular deformation. To address these constraints, we developed an innovative, wearable, all-fiber-structured electrochemical sensor. Our composite sensor incorporates polyurethane (PU) fibers prepared via electrospinning as electrode substrates to achieve excellent adaptability. Electrospun PU nanofiber films with gold layers shaped via thermal evaporation are used as base electrodes with exemplary conductivity and electrochemical catalytic attributes. To achieve glucose monitoring, gold nanofibers functionalized by gold nanoflakes (AuNFs) and glucose oxidase (GOx) serve as the working electrode, while Pt nanofibers and Ag/AgCl nanofibers serve as the counter and reference electrode. The acrylamide-sodium alginate double-network hydrogel synthesized on electrospun PU fibers serves as the adhesive and substance-transferring layer between the electrodes. The all-fiber electrochemical sensor is assembled layer-by-layer to form a robust structure. Given the stretchability of PU nanofibers coupled with a high specific surface area, the manufactured porous microneedle glucose sensor exhibits enhanced stretchability, superior sensitivity at 31.94 μA (lg(mM))-1 cm-2, a broad detection range (1-30 mM), and a significantly low detection limit (1 mM, S/N = 3), as well as satisfactory biocompatibility. Therefore, the novel electrochemical microneedle design is well-suited for wearable or even implantable continuous monitoring applications, thereby showing promising significant potential within the global arena of wearable medical technology.