Transduction of Amine-Phosphate Supramolecular Interactions and Biosensing of Acetylcholine through PEDOT-Polyamine Organic Electrochemical Transistors

MONTERO-JIMENEZ, MARJORIE; LUGLI-ARROYO, JUAN; FENOY, GONZALO E.; PICCININI, ESTEBAN; KNOLL, WOLFGANG; MARMISOLLÉ, WALDEMAR A.; AZZARONI, OMAR

ACS APPLIED MATERIALS & INTERFACES

AMER CHEMICAL SOC

Año: 2023

1944-8244

Organic electrochemical transistors (OECTs) are important devices for the development of flexible and wearable sensors due to their flexibility, low power consumption, sensitivity, selectivity, ease of fabrication, and compatibility with other flexible materials. These features enable the creation of comfortable, versatile, and efficient portable devices that can monitor and detect a wide range of parameters for various applications. Herein, we present OECTs based on PEDOT-polyamine thin films for the selective monitoring of phosphate-containing compounds. Our findings reveal that supramolecular single phosphate-amino interaction induces higher changes in the OECT response compared to ATP-amino interactions, even at submillimolar concentrations. The steric character of binding anions plays a crucial role in OECT sensing, resulting in a smaller shift in maximum transconductance voltage and threshold voltage for bulkier binding species. The OECT response reflects not only the polymer/solution interface but also events within the conducting polymer film, where ion transport and concentration are affected by the ion size. Additionally, the investigation of enzyme immobilization reveals the influence of phosphate species on the assembly behavior of acetylcholinesterase (AchE) on PEDOT-PAH OECTs, with increasing phosphate concentrations leading to reduced enzyme anchoring. These findings contribute to the understanding of the mechanisms of OECT sensing and highlight the importance of careful design and optimization of the biosensor interface construction for diverse sensing applications.