摘要
为改善聚酰亚胺(PI)的溶解性和可融性,合成了两种含三氟甲基的芳香二胺单体,并以3,3′,4,4′-二苯甲酮四羧酸二酐(BTDA)作为二酐单体,选用端氨丙基聚二甲基硅氧烷(APPS)作为柔性链单元,间氨基苯乙炔(APA)作为活性封端剂,制备得到一系列加成型热固性含氟聚(酰亚胺-硅氧烷)共聚树脂(ABIS)。用核磁共振氢谱和红外表征ABIS的结构,并研究其溶解性、流变特性和固化后的热稳定性。用溶液成膜法制备了ABIS薄膜,研究了薄膜的物理特性。用热压法以T300碳布作为增强体制备了ABIS树脂基复合材料(T300CF/ABIS),并对其力学性能进行了探究。结果表明:硅氧烷链段和三氟甲基的引入可以显著提升PI树脂体系的流动性和溶解性。引入含氟芳香二胺后虽然ABIS固化树脂的5%热失重温度(T_(d5))有所降低,但仍超过425℃,800℃下的残留率(Y_(r800℃))达到26%。ABIS薄膜的拉伸强度和断裂伸长率分别高达15.8 MPa和65.3%,在40~107 Hz下的介电常数(ε)和介质损耗因数(tanδ)分别约为3.21和0.01且基本不变,超纯水在ABIS膜表面的接触角为94°。T300CF/ABIS复合材料的弯曲强度和层间剪切强度(ILSS)分别高达137.6 MPa和16.6 MPa。本研究制备的ABIS树脂有望在微电子器件和柔性防热复合材料中获得应用。
In order to improve the solubility and meltability of polyimide(PI),a series of addition thermosetting fluorinated poly(imide-siloxane)copolymer resins(ABIS)were prepared from two kinds of synthesized trifluoromethyl-containing aromatic diamine monomers and 3,3′,4,4′-benzophenone tetracarboxylic acid dianhydride(BTDA),besides,aminopropylterminated polydimethylsiloxane(APPS)was chosen as flexible segment,and 3-aminophenyl acetylene(APA)was used as reactive end-capping agent.The structure of ABISs were characterized by proton nuclear magnetic resonance spectroscopy(1H NMR)and Fourier transformation infrared spectroscopy(FTIR).The solubility,rheological behavior of ABIS and the thermal stability of the cured ABIS were further studied.Moreover,ABIS films were prepared by solution filming,and their physical properties were studied.ABIS resin matrix composites(T300CF/ABIS)were prepared by hot pressing using T300 carbon cloth as reinforcement,and their mechanical properties were also tested.The results show that the introduction of siloxane segment and trifluoromethyl group can significantly increase the flowability and solubility of PI resin systems.The introduction of fluorinated diamine decreases the 5%weight loss temperature(T_(d5))of the cured ABIS,but its Td5 is still higher than 425℃.At the same time,the residual yield at 800℃(Y_(r800℃))of ABIS resins reach 26%.The tensile strength and elongation at break of ABIS films are as high as 15.8 MPa and 65.3%,respectively.In the frequency range of 40 Hz−107 Hz,the dielectric constant(ε)and dielectric loss factor(tanδ)of the PI films are 3.21 and 0.01,respectively,which keep unchanged basically.The contact angle of water on the cured ABIS film is 94°.The flexural strength and interlaminar shear strength(ILSS)of T300CF/ABIS composites can be 137.6 MPa and 16.6 MPa,respectively.The synthesized ABIS resin has promising applications in microelectronic devices and flexible heat-protective composites.
作者
喻文章
袁荞龙
YU Wenzhang;YUAN Qiaolong(Key Laboratory of Specially Functional Polymeric Materials and Related Technology of the Ministry of Education,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China)
出处
《绝缘材料》
CAS
北大核心
2024年第10期68-77,共10页
Insulating Materials
基金
中央高校基本科研业务费专项资金资助(JKD01241701)。
