基于聚亚胺的仿生复合材料制备及性能研究

发布时间：2018-01-16 17:34

本文关键词：基于聚亚胺的仿生复合材料制备及性能研究　出处：《吉林大学》2017年博士论文　论文类型：学位论文

【摘要】：聚亚胺,也被称为希夫碱,是一种新型的热固性聚合物,具有可塑性、可循环性、可自修复性等一系列非常独特的性质,因此引起了广泛的关注和研究。现有关于聚亚胺的研究主要是将少量的聚亚胺材料添加进碳材料或其他聚合物制备复合材料,而基于聚亚胺自身的增强复合材料却鲜有报道。本文合成了性能不同的聚亚胺基底材料,并基于动态共价化学反应制备了碳酸钙(CaCO_3)增强聚亚胺仿生复合材料、二氧化锆(ZrO_2)增强聚亚胺纳米复合材料和软硬相间聚亚胺仿生复合材料。对上述聚亚胺基底材料和三种复合材料分别进行了基本理化性能的表征和机械性能、热学性能的检测。本文由不同的二醛(对苯二甲醛和戊二醛)和二乙烯三胺、三乙烯四胺制备了两种不同的聚亚胺基底材料,分别为含对苯二甲醛的PI-H和含戊二醛的PI-S。首先,PI-H和PI-S均具有良好的耐常见有机溶剂腐蚀性和46%左右的吸水率,而在其他性能上表现不同。但整体而言,PI-H和PI-S具有一些聚亚胺材料独有的特性:加热时具有可塑性,可循环使用性,且具有自修复性质。而两种聚亚胺材料的各项机械性能保持较高数值,能与常见的塑料相媲美。本文将CaCO_3颗粒以不同的比例添加进聚亚胺基底粉末中,制备了一系列CaCO_3增强的聚亚胺仿生复合材料。由机械测试结果可知,CaCO_3增强的仿生聚亚胺复合材料的拉伸强度、韧性、弯曲强度和抗冲击强度等机械性能相对于聚亚胺基底材料都有大幅度提高。特需指出,CaCO_3增强的仿生聚亚胺复合材料良好的结合了拉伸强度和韧性,使得两者被同时增强。CaCO_3增强的仿生聚亚胺复合材料的不同机械性能达到最优值时需要添加CaCO_3颗粒的量不同。同时,添加CaCO_3颗粒还对聚亚胺基底材料的热稳定性有一定程度的提升。本文还尝试将ZrO_2纳米粒子按不同的比例掺入聚亚胺基底材料中,通过X射线衍射(XRD)和傅里叶红外(FT-IR)结果确认成功制备了一系列ZrO_2增强的聚亚胺纳米复合材料。ZrO_2增强的聚亚胺纳米复合材料的拉伸强度、韧性、抗冲击强度、弯曲强度、断裂伸长率等各项机械性能相对于聚亚胺基底均被显著提高,但与添加CaCO_3颗粒的情况类似,ZrO_2增强的聚亚胺纳米复合材料达到不同机械性能最大值时对应的Zr O_2纳米粒子添加量不同。不同于常规的无机-有机复合材料,Zr O_2增强的聚亚胺纳米复合材料的拉伸强度和韧性在相同的ZrO_2添加量下能被同时增大。同样,添加ZrO_2纳米粒子还能对复合材料的热稳定性有一定的提高。此外,本文利用亚胺的动态共价化学复分解反应,基于硬度不同的PI-H和PI-S两种聚亚胺基底材料,通过简便的热压方法制备了一系列软硬相间聚亚胺仿生复合材料。本文制备的软硬相间聚亚胺仿生复合材料可以实现两种基底材料PI-H和PI-S从0%到100%的任意比例混合,并能产生协同作用。当PI-S添加量为25%时,软硬相间聚亚胺仿生复合材料的摩擦系数、抗冲击强度和拉伸弹性模量均出现极值。特需指出,软硬相间仿生复合材料摩擦系数极值点所对应的PI-S添加量不随摩擦速度改变而改变,但却随着负载变化而变化,说明对于软硬相间复合材料摩擦性能起决定性作用的工况条件主要是负载。无论是在摩擦测试、抗冲击测试或是原位拉伸测试中,软硬相间聚亚胺仿生复合材料表现出的特性都是结合了PI-H和PI-S各自的性质。所以当PI-S以适当比例(25%)添加时,软硬相间聚亚胺仿生复合材料的不同机械性能,包括摩擦系数、抗冲击强度和拉伸弹性模量均出现最优值,并都优于两种聚亚胺基底材料。本文为日后制备基于聚亚胺的复合材料提供了有效的参考和新的方法,并且也为聚合物复合材料中不同组分添加比例实现0-100%的任意比例调整提供了新的借鉴。同时,本文展示了一种价格低廉,操作简便的制备聚亚胺增强复合材料的方法,为制备基于聚亚胺的增强复合材料提供了新思路,也为拓展聚亚胺材料的应用提供了更多的可能。
[Abstract]:Polyimide, also known as the Schiff base, is a kind of new thermosetting polymers, has plasticity, can be recycled, can self repair and a series of unique properties, it has aroused widespread concern and research. The existing research on polyimide is mainly the polyimide material adding a small amount of carbon. Preparation of composite materials or other polymer material, polyimide and its reinforced composite materials are rarely reported. Based on polyimide substrate materials with different properties have been synthesized, and dynamic covalent chemical reaction based on the preparation of calcium carbonate (CaCO_3) reinforced polyimide biomimetic composite materials, two zirconia (ZrO_2) reinforced polyimide nano composite materials and soft hard alternate polyimide biomimetic composite materials. The polyimide substrate material and three kinds of composites were studied and mechanical properties of basic physicochemical properties, thermal properties. This paper consists of detection Two different aldehydes (two of benzene formaldehyde and glutaraldehyde) and two ethylene amine three, three ethylene four amine was prepared by two different polyimide substrates, respectively containing two of benzene formaldehyde and glutaraldehyde containing PI-H PI-S. first, PI-H and PI-S have good resistance to water absorption of common organic solvent resistance and the rate of about 46%, while the performance of the other properties are different. But on the whole, PI-H and PI-S have some unique properties of polyimide materials: plastic heating, recycling, and self repairing properties. And two kinds of all the mechanical properties of polyimide materials can maintain a higher value, can compared with common plastic. The CaCO_3 particles with different proportion of added polyimide substrate powder, a series of polyimide biomimetic composites reinforced by CaCO_3 was prepared. The mechanical test results show that the bionic CaCO_3 reinforced polyimide composite material The tensile strength, toughness, mechanical properties, bending strength and impact strength relative to the polyimide substrate materials are greatly improved. The special CaCO_3 pointed out that the bionic reinforced polyimide composite material with good tensile strength and toughness, the amount of different mechanical properties reached the optimal value when the need to add CaCO_3 particles was also enhanced to make two bionic.CaCO_3 reinforced polyimide composites. At the same time, improved to a certain degree of addition of CaCO_3 particles of polyimide substrate material thermal stability. This paper also attempts to ZrO_2 nanoparticles with different proportion doped polyimide substrate material, by means of X ray diffraction (XRD) and Fourier transform infrared (FT-IR) results confirm a series of ZrO_2 reinforced poly.ZrO_2 imine nanometer composites reinforced polyimide nano composite material tensile strength, prepared toughness, impact strength, bending The strength, elongation and other mechanical properties of the polyimide substrate were compared with similar but significantly increased with the addition of CaCO_3 particles, polyimide nano composite material to different mechanical properties Zr content corresponding to the maximum value of O_2 nanoparticles enhanced ZrO_2 different. Different from the conventional inorganic organic composite materials, dosage of Zr O_2 reinforced polyimide nano composite material tensile strength and toughness under the same ZrO_2 can be increased at the same time. Similarly, added could improve the thermal stability of ZrO_2 nanoparticles but also on composite materials. In addition, this paper uses dynamic covalent chemistry imine metathesis reaction, two different hardness PI-H and PI-S polyimide substrate based on the simple method of preparation by pressing a series of hard and soft white polyimide biomimetic composite materials. In this paper, the preparation of polyimide composite bionic hard and soft white The material can achieve two kinds of base materials of PI-H and PI-S to any proportion of 100% from 0% mixed, and can produce synergistic effect. When the amount of PI-S is 25%, the friction coefficient of soft and hard alternated polyimide biomimetic composites, impact strength and tensile modulus were extreme. Special notes, hard and soft white biomimetic composite friction the corresponding coefficient of the extreme points of the addition of PI-S did not change with the change of friction speed, but as the load changes, that play a decisive role on the friction performance of composite hard and soft white conditions is the main load. Whether in the friction test, impact test or in-situ tensile test, hard and soft white polyimino bionic the composite materials exhibit all the characteristics of the combination of PI-H and PI-S of their respective properties. So when PI-S in proper proportion (25%) is added, hard and soft white polyimide composites of different bionic The mechanical properties, including friction coefficient, impact strength and tensile modulus were the optimal value, and is better than the two kinds of polyimide substrate material. The day after the preparation of composite polyimide based on reference effective and new methods, and also for the different components of polymer composite materials in proportion to achieve any ratio adjustment of 0-100% provides a new reference. At the same time, this paper presents a low price, simple preparation of polyimide reinforced composite method, provides a new idea for the preparation of composite materials based on polyimide, provides more possibilities for the development and application of polyimide materials.

【学位授予单位】：吉林大学
【学位级别】：博士
【学位授予年份】：2017
【分类号】：TQ317;TB33

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