Li Peiyun, Shi Junwei, Lei Yuqiu, Huang Zhen, Lei Ting
Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, School of Materials Science and Engineering, Peking University, Beijing, 100871, China.
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
Nat Commun. 2022 Oct 10;13(1):5970. doi: 10.1038/s41467-022-33553-w.
High-performance n-type organic electrochemical transistors (OECTs) are essential for logic circuits and sensors. However, the performances of n-type OECTs lag far behind that of p-type ones. Conventional wisdom posits that the LUMO energy level dictates the n-type performance. Herein, we show that engineering the doped state is more critical for n-type OECT polymers. By balancing more charges to the donor moiety, we could effectively switch a p-type polymer to high-performance n-type material. Based on this concept, the polymer, P(gTDPP2FT), exhibits a record high n-type OECT performance with μC* of 54.8 F cm V s, mobility of 0.35 cm V s, and response speed of τ/τ = 1.75/0.15 ms. Calculations and comparison studies show that the conversion is primarily due to the more uniform charges, stabilized negative polaron, enhanced conformation, and backbone planarity at negatively charged states. Our work highlights the critical role of understanding and engineering polymers' doped states.
高性能n型有机电化学晶体管（OECT）对于逻辑电路和传感器至关重要。然而，n型OECT的性能远远落后于p型。传统观点认为，最低未占分子轨道（LUMO）能级决定了n型性能。在此，我们表明，对于n型OECT聚合物，调控掺杂态更为关键。通过向供体部分平衡更多电荷，我们可以有效地将p型聚合物转变为高性能n型材料。基于这一概念，聚合物P(gTDPP2FT)展现出创纪录的高n型OECT性能，其电容率为54.8 F cm V s，迁移率为0.35 cm V s，响应速度为τ/τ = 1.75/0.15 ms。计算和对比研究表明，这种转变主要归因于在负电荷状态下更均匀的电荷、稳定的负极化子、增强的构象和主链平面性。我们的工作突出了理解和调控聚合物掺杂态的关键作用。
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