Despite containing attractive redox-functional groups
in their
structure, research on radical polymers (RPs) and their integration
into biosensing applications remains limited. Herein, we propose a
study on integrating newly synthesized conjugated RP (BTMP-EDOT) with
conventional conjugated polymer (P3MEET) systems, employing them as
the active channel material in organic electrochemical transistor
(OECT)-based biosensors designed for detecting dopamine (DA). Through
precise blend composition adjustment, the optimized OECT exhibits
a volumetric capacitance value (C*) of 243 F cm–3 and a maximum transconductance (g
m) of ∼400 mS. Moreover, we achieved an exceptional
clinical-level detection limit for DA at 1 pM and remarkable ultraspecificity,
even in the presence of a large excess of interferents. The highly
sensitive and selective DA biosensing performance is achieved through
meticulous design, which involves harnessing the redox activity of
TEMPO active sites to enhance ion penetration into the bulk channel
film and engineering a synergistic inter- and intramolecular π-orbital
overlap between the primary constituents to facilitate efficient electronic
transport along and between the polymer chains. Furthermore, our proposed
design concept, coupled with CRP structure modification, could enable
the development of OECTs with exceptional performance tailored for
low-cost and disposable DA biosensing applications.