聚亞醯胺複合材料之製備與特性研究

Abstract

本論文利用成功地以一步法製備出可溶性聚亞醯胺薄膜，主要是 使用雙酸酐Bicyclo[2.2.2]oct-7-ene-2,3,5,6-tetracarboxylic Dianhydride (BCDA)及雙胺4,4'-Diaminodiphenyl Ether(ODA)製備出可溶性聚亞 醯胺。本論文分為二個研究部分，第一部分為聚亞醯胺/二氧化矽混 成薄膜，探討二氧化矽加入之後對整體聚亞醯胺性質之影響，經由光 學性質、熱性質及表面型態分析後我們得知，其薄膜穿透度可達80 %以上，玻璃轉移溫度可達380℃，熱膨脹係數由42.6ppm/℃降低至 35.5 ppm/℃，降低的幅度高達17%。 第二部分的研究為聚亞醯胺/甲酸銨混成薄膜，研究中針對此混成 薄膜之光學性質、熱性質、機械性質、介電特性等作一系列探討後可 發現，聚亞醯胺薄膜可藉由導入甲酸銨，加熱之後產生微孔洞，進而 達到增加自由體積，使介電常數下降11.5%，熱膨脹係數下降8.15%， 且加入的甲酸銨並不破壞聚亞醯胺優異的熱性質，而儲存模數也可提 升12.7%。

Soluble hybrid films have been successfully fabricated by one-step process. The soluble polyimide (PI) were prepared by the reaction of Bicyclo[2.2.2]oct-7-ene-2,3,5,6-tetracarboxylic dianhydride (BCDA) and 4,4'-Diaminodiphenyl Ether (ODA) in m-cresol at 70~180℃. The main studies of this dissertation were divided into two parts. The first part includes: synthesis and characteristic analysis of polyimide /SiO2 hybrid films. The PI/SiO2 hybrid films exhibit light transmittance higher than 80%, glass transition temperatures (Tg) increased to 380℃ and thermal expansion coefficient (CTE) down from 42.6ppm/℃ to 35.5ppm/℃. The CTE of PI/SiO2 hybrid films lower approximately 17% than that of the pristine PI film.

The second part of this thesis covers the effect of ammonium formate contents in the Polyimide/ammonium formate hybrid films on the optics properties, thermal properties, dynamic mechanical properties,dielectric constants. Polyimide hybrid films doped with the ammonium formate cause the formation of the tiny hole inside polyimide films. The ammonium formate promotes the free volume content by the gas formation of NH3、H2O and CO during imidization. The dielectric constants and thermal expansion coefficiency (CTE) were decreased 11.5% and 8.2%, respectively. However, increasing the ammonium formate contents does not deteriorate ate the polyimide excellent thermal properties surprisingly the storage modulus was enhanced 12.7%.