本論文研究利用一步法合成製備有機可溶性聚醯亞胺 (PI-1 及 PI-2) ，以此為基材結合功能性無機材料並搭配各種低溫製程，製備功能性聚醯亞胺複合材料。本論文研究主要分為四部分。
本論文研究的第一部分是合成製備有機可溶聚醯亞胺，PI-1 結構由 6F-OH diamine 及 ODPA 所組成，PI-2 則由 6F-OH diamine、ODA 及 ODPA 組成，兩者具有良好的溶解性因而可溶於常見有機溶劑，並兼具高熱穩定性，在熱重量損失達 10% 時，PI-1 及 PI-2 熱裂解溫度 Td 皆接近 515 °C。
本論文研究的第二部分是製備表面導電聚醯亞胺複合材料，並探討含有不同循環噴塗次數的 silver nanowire (AgNW) 及 carbon nanotube (CNT) 對於 PI 基內埋式表面電極導電性質的影響及其經由循環彎曲後電性的變化。將 PI-1 藉由液滴塗佈方式披覆於以噴塗方式所建構含有 AgNWs 及 CNTs 的導電網絡，最後在 PI-1 基材表層內部形成一層導電複合層的內埋式表面電極。可撓性的 CNT/PI 及 AgNW/PI 表面電極經由 30 次循環噴塗後，可獲得高導電率，分別為 6.3 S/cm 及 100 S/cm。除此之外也具有較好的彎曲耐久性， 即使經由 1200 循環彎曲後仍保持其導電穩定性。對比發現，採用 ITO 披覆的 ITO/PI 及 ITO/AgNW/PI 電極在循環彎曲下會造成嚴重的導電性劣化。
本論文研究的第三部分是製備高介電聚醯亞胺複合材料，並探討添加不同體積含量與不同改質處理的市售純鈦酸鋇及自己合成的多重摻雜鈦酸鋇 (Alfa-BT 與 SS-BT) 對於 Organosoluble PI/ceramic 混成複合膜介電性質之影響。藉由 6F-OH diamine、ODA 及 ODPA 合成製備出高介電聚醯亞胺 (PI-2) ，此 PI-2 介電常數為 K=7.4，並以此為基材分別導入體積含量達 50 vol% 的 Alfa-BT 與 SS-BT ，隨後利用網印方式建構複合薄膜，並探討其介電性質的變化。為了改善填充材於基材中聚集的行為，利用球磨處裡使顆粒尺寸均勻與細化，並利用過氧化氫 (H2O2) 氧化及接枝矽烷界面耦合劑 (3-glycidoxypropyltrimethoxysilane, GPTMS) 方式對鈦酸鋇表面進行改質。PI/SS-BT 複合材料在鈦酸鋇含量到達 50 vol% 時，具有最高的介電常數 K=52。然而，SS-BT 對於複合材料介電常數的貢獻能力，隨著填充材表面改質 OH 基團而削弱。
本論文研究的第四部分是製備導熱聚醯亞胺複合材料，並探討添加不同體積含量的 BN 及 (BN+AlN) 對於 Organosoluble PI/ceramic 混成複合膜熱導性質之影響。利用有機可溶 PI-1 為基材，分別導入體積分率達 0.6 的市售 BN 及 AlN，接著利用溶液澆鑄方式在室溫下形成薄膜，並探討其導熱性質的變化。BN 顆粒表面經由預包覆處理後可減緩沈降速度，避免相分離問題。緻密且具有可撓性的 PI/BN 複合膜經由 200 °C 乾燥處理後，在 BN 體積含量達到 60% 時，導熱係數達到 K=2.3 W/m-K，相較於純 PI-1 的 0.13 w/m-K，PI/BN 有較高熱導係數。另一方面，在 PI/(BN+AlN) 複合膜這個案例，含有較高含量 AlN 的複合膜由於具有許多孔洞，因此造成熱傳導性質下降。

In this thesis, our functional polyimide composites were prepared by mixing organosoluble polyimide derived from one-step polymerization with inorganic fillers at lower temperature to fabricate composite films. This study was divided into four parts.
The first part is to synthesize organosoluble, transparent, and flexible polyimides. Our polyimides were prepared in two different approaches. The first polyimide (PI-1) of ODPA/6F-OH diamine was prepared from dianhydride (ODPA) and 6F-OH diamine. The second copolyimide (PI-2) of ODPA/6F-OH diamine/ODA was synthesized from two kinds of diamines of 6F-OH and ODA, with dianhydride ODPA. Our polyimides with good organosolubility can be dissolved in common solvents and display high thermo-oxdative stability. The decomposition temperature (Td) at 10 wt% weight loss was ~515 °C for both polyimides.
The second part is to prepare polyimide sheets with embedded-type surface electrodes. This surface-conductive polyimides containing silver nanowires (AgNW) and carbon nanotube (CNT) as conductive fillers and PI-1 as a matrix were investigated for their electrical conductivity and electrical durability under cyclic bending. Our PI-based composite electrodes with CNT and AgNW as conductive fillers were prepared by spraying CNT and AgNW stock solutions into conductive networks, followed by drop coating a PI layer to form the embedded-type surface electrodes, where a conductive composite layer was formed on a flexible PI substrate. The CNT- and AgNW-based surface electrodes on the PI substrates not only had high electrical conductivity of 6.3 and 100 S/cm, respectively, after 30 spraying cycles but also kept electrical stability after more than 1200 bending tests. For a comparative purpose, the ITO-coated ITO/PI and ITO/AgNW/PI had severe electrical failure under cyclic bending.
The third part is to prepare high dielectric polyimides, our polyimide/BaTiO3 composites with different filler contents and types of treated ceramic powders were prepared and under investigated for their dielectric performance. Our PI-2 matrix constituted by ODPA/6F-OH diamine/ODA showed a higher dielectric constant (K) of 7.4. Ceramic fillers up to a volume percentage of 50% were mixed with polyimide to form slurry, followed by screen-printing into composite thin films and investigating their dielectric properties. In order to overcome the aggregation problems for the fillers in a PI-2 matrix, BaTiO3 fillers were underwent a particle-size refinement treatment by planetary ball milling and surface modifications by the oxidation of hydrogen peroxide and by grafting with a coupling agent of 3-glycidoxypropyltrimethoxysilane (GPTMS). The highest K value obtained for the PI-2/SS-BT hybrid composites was 52 at a 50 vol% filler content. However, the advantage of SS-BT in dielectricity of composites is easily taken away by a surface modification with the OH group covered on fillers.
The fourth part is to prepare thermal conductive polyimide composites. Our organosoluble polyimide/ceramic composites with different BN or (BN+AlN) contents were under investigation for their thermal conductivity performance. The commercially available BN and AlN fillers up to a volume ratio of 0.6 were added to the polyimide to form a slurry, followed by cast-coating into composte films under room temperature and measuring their thermal conductivities. BN powders needed a surface pre-coating treatment to avoid sedimentation. The dense and flexible PI/BN composite films, after a drying treatment at 200°C, showed high thermal conductivity of 2.3 W/m-K at a BN volume ratio of 60%, as compared with 0.13 W/m-K for our pure polyimide. However, in the case of PI/(BN+AlN) composite films, the performance of thermal conductivity degraded because the films became highly porous at the higher AlN content.

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