The development of high-performance polymer mixed ionic–electronic conductors (PMIECs) is critical for advancing organic electrochemical transistors (OECTs). While the field has been dominated by linearly conjugated polymers, cross-conjugated systems represent a vast and largely unexplored materials platform. Their distinctive optical, electronic, and tailorable redox characteristics endow them with considerable, yet underutilized, potential for the development of a range of OECT applications. In this work, we designed and synthesized two donor–acceptor (D–A) polymers, P(TIDPg-TVT) and P(TIDPg-CNTVT), based on a planar, hydrogen-bond-locked cross-conjugated acceptor (TIDP). P(TIDPg-TVT) exhibited n-type-dominant ambipolar transport coupled with high operational stability, achieving an n-type μC* of 3.25 F cm–1 V–1 s–1. The cyanofunctionalized polymer P(TIDPg-CNTVT) displayed pronounced n-type characteristics, achieving a high μC* of 4.93 F cm–1 V–1 s–1 along with efficient doping. Leveraging these polymers as the active layer, complementary OECT inverters were fabricated and demonstrated high voltage gains. This work successfully validates cross-conjugation as a versatile design paradigm for high-performance PMIECs, thereby providing a molecular engineering strategy to realize balanced ionic and electronic transport, which is critical for the development of high-performance organic bioelectronic devices.
Wang et al. (Fri,) studied this question.