Construction of Highly Active Interfaces on Screen-Printed Carbon Electrodes via Controllable Electrochemical Exfoliation for High-Performance Flexible Enzyme-Free Glucose Sensing

TL;DR

Researchers developed a flexible glucose sensor using a new method to improve electrode performance for wearable health monitoring.

Contribution

A controllable electrochemical exfoliation method is introduced to enhance electrode interfaces for high-performance enzyme-free glucose sensing.

Findings

Electrochemical exfoliation increases electrode surface area and introduces oxygen-containing groups, reducing charge transfer resistance.

Optimized exfoliation with 150 cycles improves AuNP deposition density by 158% and reduces particle size to 125 nm.

The resulting sensor achieves high sensitivity, low detection limit, and good mechanical flexibility for glucose detection.

Abstract

Enzyme-free flexible glucose sensors hold great promise in the field of wearable health monitoring. However, their performance is limited by the balance between the catalytic interface activity and stability. This paper reports a strategy for interface gradient roughening of screen-printed carbon electrodes (SPCE) via controllable electrochemical exfoliation (EE). It systematically reveals the inherent relationships among the degree of EE treatment, electrode morphology, surface chemistry, and electrochemical performance. On this basis, the deposition of gold nanoparticles (AuNPs) with high density and uniform distribution is achieved, and a high-performance flexible enzyme-free glucose sensor is constructed. The study finds that EE treatment can significantly increase the true surface area of the electrode and introduce abundant oxygen-containing functional groups, thus effectively reducing the charge transfer resistance. Nevertheless, excessive exfoliation leads to the degradation of the conductive network, indicating the existence of a critical “performance window”. The EE-SPCE optimized with 150 cycles has both a high active area and good electrical conductivity, providing an ideal deposition substrate for AuNPs, increasing their distribution density by approximately 158% and reducing the average particle size to 125 nm. The fabricated AuNPs/EE-SPCE sensor exhibits excellent performance in glucose detection: it has a high sensitivity of 550.766 μA·mM−1·cm−2 in the range of 0.1–3 mM, a detection limit of 0.0998 mM, a wide linear range, excellent selectivity, long-term stability, and good mechanical flexibility. This research not only develops an efficient and scalable method for constructing flexible sensing interfaces but also clarifies the trade-off relationship among “roughening–conductivity–catalytic performance” at the mechanistic level, providing an important theoretical basis and a general strategy for rationally designing high-performance flexible electrochemical devices.

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