导热高分子材料具有重量轻、比强度和模量高、易加工、化学稳定性优异和成本低等优点，在5G通信、雷达技术、显示器屏幕以及高集成电路等领域得到了广泛的应用。但是，高分子材料由于其本身微观分子链结构的关系，导热系数一般都在0.1-0.3 W/m·K之间，很难满足实际生产需求。因此，兼具高导热性和优异拉伸强度的高分子导热材料的设计和研发具有重要的研究意义。本论文从聚合物微观结构出发，将刚性取向有序的液晶结构引入到聚合物微观结构上来，借以改善聚合物分子链的聚集形态，在聚合物体系内引入规整的微观液晶有序区，形成高效且连续的导热通路。本论文系统地研究了液晶环氧单体结构、含量以及聚合物基体分子链结构等对液晶环氧单体/环氧聚合物分散膜内分子链有序排列的影响以及导热性能的影响，并通过多物理场耦合分析软件COMSOL Multiphysics建立液晶环氧单体/环氧聚合物分散膜的最佳参数导热模型，进一步验证了液晶环氧单体/环氧聚合物分散膜的导热机理。本论文的主要研究内容如下：

（1）设计和合成了两种近晶相液晶环氧单体4,4’-双（2,3-环氧基丙氧基）联苯（LCEM₁）和4,4’-（缩水甘油基）苯甲酸联苯二酚酯（LCEM₂）。结果表明：两种液晶环氧单体的熔点分别达到128 ºC和240 ºC，LCEM₁在XRD小角区3.56º和6.77º，呈现出液晶的小板块织构，LCEM₂在小角区4.78º和8.42º都出现强烈的衍射峰，呈现出液晶的焦锥织构，LCEM₁和LCEM₂均呈现高有序度，且都为近晶相液晶单体。

（2）使用硫醇固化剂对环氧单体进行固化得到环氧聚合物溶液，将含有刚性结构的液晶环氧单体（LCEM₁和LCEM₂）分散于环氧聚合物溶液中，采用溶液浇铸和高压电场取向成型的方法制备液晶环氧单体/环氧聚合物分散膜（LCEF₁和LCEF₂）。导热系数测试结果表明：当LCEM₁含量为30 wt%时，将LCEM₁均匀分散在LCEF₁中形成层状有序结构，LCEF₁的导热系数达到1.27 W/m·K，是纯Epoxy-thiol膜导热系数的4.5倍高（纯Epoxy-thiol膜导热系数为0.28 W/m·K）。当LCEM₂含量为30 wt%时，将LCEM₂均匀分散在LCEF₂中形成有序聚集结构，LCEF₂的导热系数达到2.36 W/m·K，是纯Epoxy-thiol分散膜的8.4倍。LCEF₂的导热系数比LCEF₁的导热系数更高的原因是LCEM₂分子结构上含有的羰基和环氧聚合物分子链上的羟基形成氢键作用，提高了分子链排列的有序度。力学性能测试结果表明：相同LCEM含量下，LCEF₂的拉伸强度要优于LCEF₁的拉伸强度。当LCEM₂的含量为10 wt%时，LCEF₂的拉伸强度可达23.8 MPa，断裂伸长率可达46.7%。

（3）在一维和二维稳定热传导方程的基础上，建立了三维稳定热传导方程，可在本征型导热高分子材料体系内传热过程中用来预测材料的导热系数。选用COMSOL Multiphysics软件对液晶环氧单体/环氧聚合物分散膜进行仿真模拟，使用软件中的三维稳态固体传热物理场模块，建立液晶环氧单体代表性体积元模型与液晶环氧单体/环氧聚合物分散膜代表性体积元模型，建立了三维稳态有限元模型，研究不同液晶环氧单体加入到环氧聚合物体系中制备得到的液晶环氧单体/环氧聚合物分散膜的热传导问题，探究温度、网格化程度和液晶单体分散程度等因素对液晶环氧单体/环氧聚合物分散膜导热性能的影响。根据理论计算模型使用软件进行数值模拟，将实验数据和软件模拟计算出的数据进行对比，发现液晶环氧单体/环氧聚合物分散膜的导热系数和实验测得的导热系数结果有较好的一致性。

Thermally conductive polymer materials have the advantages of light weight, high specific strength and modulus, easy processing, excellent chemical stability and low cost. They have been widely used in 5G communication, radar technology, display screen and high integrated circuit. However, the thermal conductivity of polymer materials is generally between 0.1-0.3 W/m·K, due to their own microscopic molecular chain structure, which is difficult to meet the actual production needs. Therefore, the design and development of polymer thermal conductive materials with high thermal conductivity and excellent tensile strength have important research significance. In this paper, starting from the polymer microstructure, the rigidly oriented ordered liquid crystal structure is introduced into the polymer microstructure to improve the aggregation morphology of the polymer molecular chain, and a regular microscopic liquid crystal ordered region is introduced into the polymer system to form an efficient and continuous thermal conduction path. In this paper, the effects of the structure and content of liquid crystal epoxy monomer and the molecular chain structure of polymer matrix on the orderly arrangement of molecular chains and thermal conductivity of liquid crystal epoxy monomer/epoxy polymer dispersion film were systematically studied. The optimal parameter thermal conductive model of liquid crystal epoxy monomer/epoxy polymer dispersion film was established by multi-physics coupling analysis software COMSOL Multiphysics, and the thermal conductive mechanism of the liquid crystal epoxy monomer/epoxy polymer dispersion film was further verified. The main research contents of this paper are as follows:

(1) Two smectic liquid crystalline epoxy monomers including 4,4’-diepoxybiphenyl (LCEM₁) and 4,4’-(glycidyl) benzoate biphenyldiol ester (LCEM₂), were designed and synthesized. The results show that the melting points of the two liquid crystal epoxy monomers reach 128 ºC and 240 ºC, respectively. LCEM₁ exhibits a small plate texture of liquid crystal in the small angle region of XRD (3.56 ºC and 6.77 ºC). LCEM₂ has strong diffraction peaks in the small angle region of XRD (4.78 ºC and 8.42 ºC), showing a focal cone texture of liquid crystal. Both LCEM₁ and LCEM₂ show high order and are smectic liquid crystal monomers.

(2) The liquid crystalline epoxy monomers (LCEM₁ and LCEM₂) with rigid structure were dispersed in the epoxy polymer solution. The liquid crystalline epoxy monomer/epoxy polymer dispersion films (LCEF₁ and LCEF₂) were prepared by solution casting and high voltage electric field orientation molding. The thermal conductivity test results show that when the LCEM₁ content is 30 wt %, LCEM₁ is uniformly dispersed in LCEF₁ to form a layered ordered structure. The thermal conductivity of LCEF₁ reaches 1.27 W/m·K, which is 4.5 times higher than that of pure Epoxy-thiol film (the thermal conductivity of pure Epoxy-thiol film is 0.28 W/m·K). When the content of LCEM₂ is 30 wt%, LCEM₂ is uniformly dispersed in LCEF₂ to form an ordered aggregation structure. The thermal conductivity of LCEF₂ reaches 2.36 W/m·K, which is 8.4 times that of pure Epoxy-thiol dispersion film. The reason why the thermal conductivity of LCEF₂ is higher than that of LCEF₁ is that the carbonyl group contained in the molecular structure of LCEM₂ and the hydroxyl group on the molecular chain of epoxy polymer form hydrogen bonding, which improves the order degree of molecular chain arrangement. The mechanical properties test results show that the tensile strength of LCEF₂ is better than that of LCEF₁ under the same LCEM content. When the content of LCEM₂ is 10 wt%, the tensile strength and the elongation at break of LCEF₂ can reach 23.8 MPa and 46.7 %, respectively.

(3) Based on the one-dimensional and two-dimensional stable thermal conductive equations, a three-dimensional stable thermal conductive equation is established, which can be used to predict the thermal conductivity of the material during the heat transfer process in the intrinsic thermal conductive polymer material system. COMSOL Multiphysics software was used to simulate the liquid crystalline epoxy monomer/epoxy polymer dispersion film. Using the three-dimensional steady-state solid heat transfer physical field module in the software, the representative volume element model of liquid crystalline epoxy monomer and the representative volume element model of liquid crystalline epoxy monomer/epoxy polymer dispersion film were established. The three-dimensional steady-state finite element model was established to study the heat conduction problem of liquid crystal crystalline epoxy monomer/epoxy polymer dispersion film prepared by adding different liquid crystalline epoxy monomers to epoxy polymer system. The effects of temperature, grid degree and dispersion degree of liquid crystal crystalline epoxy monomer on the thermal conductivity of liquid crystalline epoxy monomer/epoxy polymer dispersion film were investigated. According to the theoretical calculation model, the numerical simulation is carried out by software. The experimental data and the data calculated by software are compared. It is found that the thermal conductivity of liquid crystalline epoxy monomer/epoxy polymer dispersion film is in good agreement with the experimental results.

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