本論文針對有機電化學電晶體（organic electrochemical transistors）的性能提升，提出兩種互補的設計策略：（1）透過引入共軛阻斷練（conjugation break spacers）調控p型共軛高分子的主鏈構型與結晶性；（2）利用具選擇性的聚噻吩衍生物分散半導體型單壁碳奈米管（s-SWCNT），構築奈米混成通道材料。第一部分中，設計並合成一系列含有共軛阻斷練單元的P型共軛高分子，探討主鏈構型與結晶性對元件表現的影響。其中，以異山梨醇酐(isosorbide)為基礎的聚合物展現優異的電化學性能，其歸一化跨導 (gm,norm ) 達3.21 S cm-1，電洞遷移率（μh）為0.839 cm2V-1 s-1，臨界電壓（Vth）穩定在–0.44 V。GIWAXS分析顯示其具高度有序的分子排列，有助於有效摻雜與長期操作穩定性。相較之下，異甘露醇酐(isomannide)與異艾杜糖酐(isoidide)等具高扭曲性的高分子則呈現較低的有序性與離子傳輸能力。第二部分則探討以聚噻吩衍生物（PQT-TE與PDCTT-2T）作為選擇性分散劑，用於分選HiPCO來源的半導體型單壁碳奈米管（s-SWCNT）。光譜分析確認其具手性選擇性：PQT-TE傾向分散(8,4)碳管，而PDCTT-2T則偏好(8,6)。將所分散之碳管薄膜以滴鍍法製成有機電化學電晶體元件後，PQT-TE與PDCTT-2T分別達到高歸一化跨導值14.9與14.5 S cm-1，並展現出優異的開關速度與100次以上之循環操作穩定性。其薄膜結構有效提升聚合物、碳管與電解質三者的界面耦合，建立一種嶄新的高效訊號傳遞通道設計。

This thesis explores two complementary strategies to enhance the performance of organic electrochemical transistors (OECTs): (1) tailoring the molecular structure of p-type conjugated polymers via conjugation break spacers (CBS), and (2) developing carbon nanotube-based hybrid channels through selective dispersion using polythiophene derivatives. In the first part, a series of p-type conjugated polymers incorporating conjugation break spacers (CBS) were synthesized to investigate the effect of backbone conformation and crystallinity on device performance. Among them, the ISB-based polymer exhibited a high normalized transconductance (gm,norm) of 3.21 S cm-1, hole mobility (μh) of 0.839 cm2 V-1 s-1, and a stable threshold voltage (Vth) of –0.44 V. GIWAXS analysis revealed enhanced structural order, contributing to efficient doping and long-term operational stability. In contrast, polymers with higher torsional distortion such as IMN and IID showed reduced order and impaired ion transport. In the second part, polythiophene-based polymers—PQT-TE and PDCTT-2T—were used as selective dispersants for semiconducting single-walled carbon nanotubes (s-SWCNT). Spectroscopic characterization confirmed chirality-specific sorting, with PQT-TE preferring (8,4) tubes and PDCTT-2T favoring (8,6). Integrated into OECT devices via drop-casting, the resulting polymer–SWCNT hybrid networks exhibited high gm,norm values of 14.9 and 14.5 S cm-1, respectively, with excellent switching speed and stable operation over 100 cycles. The hybrid architecture improved interfacial coupling among polymer, nanotube, and electrolyte, forming a new channel structure optimized for efficient signal transduction.

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