Dual-mode All-PEDOT:PSS Organic Electrochemical Transistors: Enzyme/Metal-free Platform for Ultrasensitive Multiplexed Biosensing of Biomarkers
摘要
Glucose, ascorbic acid (AA), uric acid (UA), and dopamine (DA) are vital biomarkers whose dynamic concentrations correlate with critical diseases; however, multiplexed detection remains challenging for conventional electrochemical sensors because of their limited sensitivity and selectivity. Here, we present a millimeter-scale all-poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) organic electrochemical transistor (OECT) platform that integrates dual-mode sensing with enzyme/metal-free operation for ultrasensitive biomarker monitoring. By engineering polycrystalline PEDOT:PSS channels via H2SO4 post-treatment, the device achieves record-high conductivity (about (2312.0±29.9) S·cm−1), maximum transconductance (about (2.82±0.12) mS), and on/off ratio (about 210.0±7.8), enabling signal amplification at low gate voltages. The dual-mode strategy combines the selectivity of electrochemistry with the sensitivity of OECTs, realizing simultaneous detection of glucose, AA, UA, and DA with clinical-level sensitivity: detection limits down to 8 nmol·L−1 (glucose), 0.5 nmol·L−1 (AA), 5 nmol·L−1 (DA), and 0.5 nmol·L−1 (UA). Validation using human urine samples yielded recovery rates of 94%–114%. This flexible sensing platform provides a new pathway for the development of wearable biosensors for precision diagnostics.