新型聚醯亞胺-二氧化矽混成材料之 製備與性質研究

Novel Polyimide-Silica Hybrids Prepared from Alkoxysilane Containing Diamine

李俊賢(Chun-hsien Lee)

指導教授 ： 鄭俊麟

中原大學/工學院/化學工程研究所/碩士(2003年)

https://doi.org/10.6840/cycu200300599

摘要

中文摘要
由於聚醯亞胺混成材料具有合成之多樣性與製備之簡單性，運用有機無機混成複合材料技術，可將無機材料優異的機械、耐熱等特性與有機材料易加工、高相容度等特性結合，而獲得具有相乘效應的效果，因此在未來的機能塗料、光電材料、電子材料及高強度複合材料等領域中具極大的應用發展潛力。
本研究主要開發二種新型雙胺單體，首先經由Grignard反應製備出具有線性烷基側鏈之芳香族雙胺單體1,1’-di-p-aminophenyl hexane (HADA)；其次，藉由醯氯反應在雙胺單體分子側鏈邊合成具有藕合無機的基團之3,5-diaminobenzamide-n-propyl triethoxylsilane (PTSDA)
。隨後二者分別與3,3-4,4-benzophenone tetracarboxylic dianhydride (BTDA)反應形成聚醯胺酸，再以高溫環化脫水製備聚醯亞胺。進而探討其熱性質與介電性質。
經由黏度的測量顯示，當雙胺結構中具有線性烷基或是藕合基團時，其側邊基團之立體障礙將會造成聚合反應的降低，因此黏度值會較低。在熱穩定性質分析，其結果顯示，摻合有SiO2粒子後之聚醯亞胺，其裂解溫度會隨著TEOS的摻合量增加而增加，且其熱裂解溫度均高於450℃。玻璃轉移溫度的量測也顯示，含有SiO2聚醯亞胺會受到分子中SiO2粒子數量的提高，造成分子鏈轉動發生困難，因此玻璃轉移溫度會上升。在介電性質測量，本實驗結果顯示，隨著TEOS摻合量的增加，其薄膜介電常數值會呈現增加的趨勢。

關鍵字

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並列摘要

Abstract
Polyimides are high-performance polymer materials with excellent thermal stability, mechanical property, and chemical resistance, etc. In this study, we synthesized two types of new diamine monomers. The 1,1’-di-p-aminophenyl hexane with linear alkyl side chain were synthesized by Grignard reaction, and the 3,5-diaminobenzamide-n-propyltriethoxylsilane with coupling side chain were synthesized by the acid chloride reaction. A series of new type of polyimides/silica hybrid materials using the sol-gel method were prepared by the 3,5-diaminobenzamide-n-propyltriethoxylsilane with 3,3’-4,4’-benzophenone tetracarboxylic dianhydride (BTDA). The polyimides were obtained by dehydrating the poly(amic acid)s in high temperature conditions, and they were characterized by 1H-NMR and IR graph.
The results showed that the viscosity is decreased by the effect of the polymer side chain and the coupling agent. The thermal properties were characterized by TGA, DSC and TMA. The BTDA-PDA/SiO2 hybrid thin films are more thermal stable than BTDA-PDA-PTSDA/SiO2 owing to the higher molecular weight. The glass transition temperature(Tg) in BTDA-PDA-PTSDA/SiO2 series are more higher than BTDA-PDA/SiO2 series because of the coupling effect between polymer chains. The coefficient of thermal expansion were decreased when the inorganic phase were increased by coupling and sol-gel effect. Moreover, the dielectric constant were increased by coupling and sol-gel effect and when the amount of TEOS increased.

並列關鍵字

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參考文獻

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