含苯并咪唑基团的聚酰亚胺树脂及其碳纤维复合材料的研究
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摘要
聚酰亚胺(PI)薄膜由于具有优异的综合性能,包括耐热性、机械性能、尺寸稳定性及电气绝缘性能而被广泛应用于高技术领域。其最为典型的应用是作为柔性基底材料使用,例如,在微电子工业中,将聚酰亚胺薄膜作为柔性印刷线路板和自粘带技术用的基底材料;PI薄膜也可以作为薄膜太阳能电池的柔性基底。在这些应用领域中,对聚酰亚胺薄膜材料的热性能、机械性能及尺寸稳定性均有较高的要求。
     本论文使用一种含有苯并咪唑基团的二胺单体2-(3-氨基苯基)-5-氨基苯并咪唑(i-DAPBI)与二酐单体进行缩聚反应,得到一系列聚酰亚胺薄膜,并对该类薄膜的热性能和机械性能进行表征。结果表明,该类薄膜具有较高的耐热性和良好的机械性能。同时,二胺单体中氨基的相对位置赋予分子链以较高的弯曲性,使该类聚酰亚胺具有较好的热塑性和较高的热膨胀系数。采用i-DAPBI和DAPBI作为二胺单体,采用苯乙炔苯酐(4-PEPA)直接封端的方法合成小分子模型化合物。同时采用i-DAPBI与不同种二酐单体(s-BPDA,a-BPDA,ODPA,BPADA)共聚,经过程序升温后制备成热塑性聚酰亚胺;另一部分同样采用4-PEPA封端,得到不同聚合度的聚酰亚胺预聚体,通过熔融压制并在370℃交联1小时,得到了热固性的聚酰亚胺薄膜,并对聚合物进行了各项性能的比较。研究表明,本文所合成的聚酰亚胺树脂是一种较好的可应用于航空航天领域的先进树脂基体。尤其是采用i-DAPBI制备的树脂具有较低的熔体黏度和较宽的加工窗口;同时固化后具有更好的热稳定性能,具有极为良好的应用潜力。在对树脂进行评价之后,选用其中的一种树脂制备了碳纤维增强的复合材料,对复合材料进行了初步评价测试,结果表明此类复合材料具有优异的力学性能,为今后制备性能更加优良的聚酰亚胺碳纤维复合材料提出了改进措施。
Polyimide (PI) films have been widely applied in high technology fields, due tothe good combination of properties, including thermal resistance, mechanicalproperties, dimensional stability and electric insulating properties. The most classicalapplication is the flexible substrate materials. For example, PI films could be used asthe substrates of the flexible printed circuit board (FPC) and tape automated bondingin the field of microelectronics; they also could be the flexible substrates of thin-filmssolar cells. High performance of PI films is required for these applications. Forinstance, when used as the substrates for FPC, Besides, CTE values should be smallerfor the application of solar cells. Common PI films have CTE values of greater than30ppm/K. Therefore, properties of PI films are required to improve to adapt to theneeds of high performance applications.
     This paper uses a benzimidazole group containing diamine monomer2-(3-amino-phenyl)-5-aminobenzimidazole and dianhydride monomer polycondensationreaction to obtain a series of polyimide film, and thermal and mechanical properties ofsuch films were characterized. The results show that the film has such high heatresistance and good mechanical properties. Meanwhile, the relative position of theamino group to give diamines of the molecular chain with high bending resistance,such that the thermoplastic polyimide has a better thermal expansion coefficient andhigher. Using i-DAPBI and DAPBI as diamine monomer, using phenylacetyleneanhydride (4-PEPA) capped directly synthesized small molecule model compounds.While using different types of i-DAPBI dianhydride monomer (s-BPDA, a-BPDA,ODPA, BPADA) copolymer, prepared after the process temperature of thethermoplastic polyimide; another part uses the same4-PEPA capped give differentdegrees of polymerization polyimide prepolymer by melt-pressed and crosslinked at 370℃1hour to obtain a polyimide film thermoset polymer and a comparison of theperformance. Studies show that this synthesized polyimide resin has reached theinternational advanced level, is a good can be applied to an advanced aerospace resinmatrix. Especially the use of a resin prepared by i-DAPBI lower melt viscosity andhas a wide processing window; simultaneously cured with better thermal stability,with a very good potential applications. After the evaluation of the resin, use of a resinprepared in which the carbon fiber reinforced composite materials, compositematerials were preliminary evaluation test results show that the composites haveexcellent mechanical properties, and more excellent performance in the future for thepreparation of poly imide carbon fiber composite material made improvements.
引文
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