Cyano-Functionalized n-Type Polymer with High Electron Mobility for High-Performance Organic Electrochemical Transistors

n-Type organic mixed ionic-electronic conductors (OMIECs) with high electron mobility are scarce and highly challenging to develop. As a result, the figure-of-merit (mu C*) of n-type organic electrochemical transistors (OECTs) lags far behind the p-type analogs, restraining the development of OECT-based low-power complementary circuits and biosensors. Here, two n-type donor-acceptor (D-A) polymers based on fused bithiophene imide dimer f-BTI2 as the acceptor unit and thienylene-vinylene-thienylene (TVT) as the donor co-unit are reported. The cyanation of TVT enables polymer f-BTI2g-TVTCN with simultaneously enhanced ion-uptake ability, film structural order, and charge-transport property. As a result, it is able to obtain a high volumetric capacitance (C*) of 170 +/- 22 F cm(-3) and a record OECT electron mobility (mu(e,OECT)) of 0.24 cm(2) V-1 s(-1) for f-BTI2g-TVTCN, subsequently achieving a state-of-the-art mu C* of 41.3 F cm(-1) V-1 s(-1) and geometry-normalized transconductance (g(m,norm)) of 12.8 S cm(-1) in n-type accumulation-mode OECTs. In contrast, only a moderate mu C* of 1.50 F cm(-1) V-1 s(-1) is measured for the non-cyanated polymer f-BTI2g-TVT. These remarkable results demonstrate the great power of cyano functionalization of polymer semiconductors in developing n-type OMIECs with substantial electron mobility in aqueous environment for high-performance n-type OECTs.

Automated summary

n-Type organic mixed ionic-electronic conductors with high electron mobility are developed, enabling the development of high-performance n-type organic electrochemical transistors. The cyano functionalization of the donor-acceptor polymers greatly enhances their ion-uptake ability, film structural order, and charge-transport property, resulting in a record electron mobility and volumetric capacitance in n-type OECTs.