Organic electrochemical transistors (OECTs) are oft-used for bioelectronic applications, and a variety of OECT channel materials have been developed in recent years. However, the majority of these materials are still limited by long-term performance and stability challenges. To resolve these issues, we implemented a next-generation design of polymers for OECTs. Specifically, diketopyrrolopyrrole (DPP) building blocks were copolymerized with propylene dioxythiophene-based (Pro-based) monomers to create a donor–acceptor-type conjugated polymer (PProDOT-DPP). These PProDOT-DPP macromolecules were synthesized using a straightforward direct arylation polymerization synthetic route. The PProDOT-DPP polymer thin film exhibited excellent electrochemical response, low oxidation potential, and high crystallinity, as evidenced by spectroelectrochemical measurements and grazing incidence wide-angle X-ray scattering measurements. Thus, the resultant polymer thin films had high charge mobility and volumetric capacitance values (i.e., μC* as high as 310 F cm^–1 V^–1 s^–1) when they were used as the active layer materials in OECT devices, which places PProDOT-DPP among the highest performing accumulation-mode OECT polymers reported to date. The performance of the PProDOT-DPP thin films was also retained for 100 cycles and over 2000 s of ON–OFF cycling, indicating the robust stability of the materials. Therefore, this effort provides a clear roadmap for the design of electrochemically active macromolecules for accumulation-mode OECTs, where crystalline acceptor cores are incorporated into an all-donor polymer. We anticipate that this will ultimately inspire future polymer designs to enable OECTs with both high electrical performance and operational stability.

中文翻译：

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设计用于稳定和高性能有机电化学晶体管的供体-受体共聚物

有机电化学晶体管 (OECT) 常用于生物电子应用，近年来已开发出多种 OECT 通道材料。然而，这些材料中的大多数仍然受到长期性能和稳定性挑战的限制。为了解决这些问题，我们实施了用于 OECT 的下一代聚合物设计。具体来说，二酮吡咯并吡咯 (DPP) 结构单元与丙烯二氧噻吩基 (Pro-based) 单体共聚以产生供体-受体型共轭聚合物 (PProDOT-DPP)。这些 PProDOT-DPP 大分子是使用直接的直接芳基化聚合合成路线合成的。PProDOT-DPP聚合物薄膜表现出优异的电化学响应、低氧化电位和高结晶度，正如光谱电化学测量和掠入射广角 X 射线散射测量所证明的那样。因此，所得聚合物薄膜具有高电荷迁移率和体积电容值（即 μC * 高达 310 F cm ^–1 V ^–1 s ^–1 )，当它们用作 OECT 器件中的有源层材料时，这使 PProDOT-DPP 成为迄今为止报道的性能最高的累积模式 OECT 聚合物之一。PProDOT-DPP 薄膜的性能也保持了 100 次循环和超过 2000 秒的开关循环，表明材料具有强大的稳定性。因此，这项工作为设计用于累积模式 OECT 的电化学活性大分子提供了清晰的路线图，其中将晶体受体核结合到全供体聚合物中。我们预计这将最终激发未来的聚合物设计，使 OECT 具有高电气性能和操作稳定性。