Construction of Highly Active Interfaces on Screen-Printed Carbon Electrodes via Controllable Electrochemical...

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.