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 electrochem...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 H_2 SO_4 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.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.52272214,52372082,52466013,52373184,and U24A20660)Jiangxi Provincial Natural Science Foundation(Nos.20242BAB26059,20232BAB204032,20252BAC200290,20252BEJ730349,and 20252BAC240326)Doctoral Start-Up Fund of Jiangxi Science&Technology Normal University(No.2024BSQD16)。
文摘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 H_2 SO_4 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.