导热聚合物因其优异的电绝缘性能、机械性能和稳定的化学性能而被广泛地应用于电路基板、界面粘接和封装检测等行业。然而，传统聚合物由于分子链排列无序导致其较低的热导率，极大地限制了其在导热/散热领域的应用。具有特殊理化特性的液晶材料，其自身有序的微观结构、优良的加工性能以及对热、电、磁等外界刺激的响应特性，显示出了在本征型导热聚合物材料领域巨大的应用前景。本论文从聚合物微观结构出发，将刚性的液晶结构引入到聚合物体系中，利用小分子液晶基元的空间位阻和有序排列特性调整聚合物分子链的无序性，实现对聚合物微观结构的有序调控。较系统地研究了液晶单体结构、含量以及聚合物主链分子结构等对液晶-聚合物分散膜的分子链的有序排列及微观有序结构的影响关系，探索了本征型导热聚合物材料的导热性能和应用价值，主要研究内容如下：

（1）利用酯化反应和醚化反应合成了两种近晶相液晶单体4,4'-二戊酸联苯酯（M₁）和4,4'-二戊氧基联苯醚（M₂）。结果表明两种液晶单体的各向同性态温度分别达到108 ºC和130 ºC，均表现出可逆的相转变行为。M₁在XRD小角区3.78º和7.64º，M₂在小角区4.28º和8.54º都出现强烈的衍射峰，两种液晶单体均具有高有序度。

（2）将含有刚性结构的液晶单体分散于聚乙烯醇（PVA）薄膜中，采用溶液浇铸和热压的方法制备具有互穿网络结构的液晶单体-PVA分散膜（P-PDLC₁和P-PDLC₂）。结果表明，当M₁含量为15 wt%时，M₁均匀分散在P-PDLC₁膜中形成层状有序结构，热导率迅速提高至1.36 W m^-1 K^-1，是纯PVA的10倍；当M₁含量为35 wt%时，P-PDLC₁膜微观形成球状有序结构，热导率提高至1.41 W m^-1 K^-1。当M₂含量为15 wt%时，M₂均匀分散在P-PDLC₂膜中形成层状有序结构，热导率提高至1.20 W m^-1 K^-1；当M₂含量增加到25 wt%时，P-PDLC₂膜微观有序性被破坏，热导率降低至0.85 W m^-1 K^-1，M₁和PVA分子链之间产生的氢键作用提高了分子链排列的有序度，P-PDLC₁膜比P-PDLC₂膜表现出更好的导热性能。

（3）将M₁均匀分散在环氧单体和硫醇固化剂的溶液中，通过聚合工艺制备了液晶-环氧聚合物分散膜（E-PDLC），研究了M₁含量和固化剂官能度对E-PDLC膜微观形貌和导热性能的影响。结果表明，三羟甲基丙烷三(3-巯基丙酸酯)（TTMP）固化的E-PDLC膜呈现出层状的穿插网络结构，在M₁含量为20 wt%时，热导率达到0.50 W m^-1 K^-1；四(3-巯基丙酸)季戊四醇酯（PETMP）固化的E-PDLC膜微观形成鳞片状网络结构，在M₁含量为30 wt%时，热导率达到0.56 W m^-1 K^-1。

（4）将M₁均匀分散在环氧单体和硫醇固化剂的溶液中，利用M₁在电场环境下有序取向的特性，通过聚合工艺制备了具有电场取向的液晶-环氧聚合物分散膜（E_V-PDLC）。研究发现，电场作用可以显著提高E_V-PDLC膜微观形貌的有序度和热导率。TTMP固化的E_V-PDLC膜在M₁含量为20 wt%和30 wt%时，样品微观形成致密且均匀的层状结构，热导率达到0.75 W m^-1 K^-1；PETMP固化体系中在M₁含量为20 wt%时，样品微观形成紧密的球状有序结构，热导率提高到0.78 W m^-1 K^-1，在M₁含量为30 wt%时，形成有序度较低的枝状结构，热导率降至0.64 W m^-1 K^-1。外加电场促进了M₁和环氧分子链的有序取向，使E_V-PDLC膜中的有序结构更加均匀和密集，对液晶分子有序排列的稳定作用也更强。

Thermal conductive polymers are widely used in many industries such as circuit substrates, interface bonding, and packaging testing due to their excellent electrical insulation properties, mechanical properties and stable chemical properties. However, traditional polymers have lower thermal conductivity due to the disorderly arrangement of molecular chains, which greatly limits their application in the field of thermal conduction/thermal dissipation. Liquid crystal materials with special physical and chemical properties have their own orderly microstructure, excellent processing properties, and response characteristics to external stimuli such as heat, electricity, and magnetism, which shows great application prospects in the field of intrinsic thermal conductive polymer materials. This paper started from the polymer microstructure to improve thermal conductivity of polymer materials. In this paper, the rigid liquid crystal structure was introduced into the polymer system, and the steric hindrance and orderly arrangement characteristics of the liquid crystal monomer was used to improve the disorder of the polymer molecular chains, achieving the regulation of the orderly arrangement of polymer molecular chains. In this paper, the influence of the structure and the content of liquid crystal monomer, and polymer backbone structure on the orderly arrangement was systematically studied and micro-ordered structure of the molecular chain of the liquid crystal polymer dispersion film was researched, exploring the thermal conductivity and application value of intrinsic thermal conductive polymer materials. The main research contents of this paper are as follows:

Two smectic liquid crystal monomers named 4,4′- Bis(valerate)biphenyl (M₁) and 4,4'-dipentoxydiphenyl ether (M₂) were synthesized by esterification reaction and etherification reaction. The results showed that the isotropic temperature of the two liquid crystal monomers reached 108 ºC and 130 ºC, respectively, and both exhibited reversible phase transition behavior. M₁ exhibited strong diffraction peaks in the small XRD area of 3.78º and 7.64º, as well as M₂ exhibited strong diffraction peaks in the small angle area of 4.28º and 8.54º. Both liquid crystal monomers possessed the high degree of order.

The liquid crystal monomers containing rigid structure were dispersed in the polyvinyl alcohol (PVA) film, and the liquid crystal monomer-PVA dispersion films with interpenetrating network structure (P-PDLC₁ and P-PDLC₂) were prepared by solution casting and hot pressing. The results showed that when the content of M₁ was 15 wt%, M₁ was uniformly dispersed in the P-PDLC₁ film to form layered ordered structures, and the thermal conductivity rapidly increased to 1.36 W m^-1 K^-1, which was 10 times higher than that of pure PVA film. When the content of M₁ was 35 wt%, the P-PDLC₁ film microscopically formed spherical ordered structures, and the thermal conductivity increased to 1.41 W m^-1 K^-1. When the content of M₂ was 15 wt%, M₂ was uniformly dispersed in the P-PDLC₂ film to form layered ordered structures, and the thermal conductivity increased to 1.20 W m^-1 K^-1. When the content of M₂ increased to 25 wt%, the microscopic order of the P-PDLC₂ film was destroyed, and the thermal conductivity reduced to 0.85 W m^-1 K^-1. The hydrogen bond between M₁ and the PVA molecular chain increased the molecular The order of chain arrangement, P-PDLC₁ film showed better thermal conductivity than P-PDLC₂ film because the hydrogen bond between M₁ and the PVA molecular chain improved the orderly arrangement of molecular chain.

M₁ was uniformly dispersed in the solution of epoxy monomer and mercaptan curing agent, and liquid crystal-epoxy polymer dispersion film (E-PDLC) was prepared by polymerization process. The effect of the content of M₁ and curing agent functionality on the microscopic morphology and thermal conductivity of E-PDLC was studied. The results showed that the E-PDLC film cured by Trimethylolpropane Tris(3-mercaptopropionate) (TTMP) exhibited layered interlaced network structures, and the thermal conductivity reached 0.50 W m^-1 K^-1 when the content of M₁ was 20 wt%. The E-PDLC film cured by Pentaerythritol Tetra(3-mercaptopropionate) (PETMP) microscopically formed scaly network structures, and when the content of M₁ was 30 wt%, the thermal conductivity reached 0.56 W m^-1 K^-1.

M₁ was uniformly dispersed in a solution of epoxy monomer and mercaptan curing agent.  Taking advantage of the orderly orientation of M₁ in an electric field environment, liquid crystal monomer-epoxy dispersion (E_V-PDLC) film with electric field orientation was prepared through a polymerization process. The study found that the electric field could significantly improve the degree of order and thermal conductivity of the micro-morphology of E_V-PDLC film. When the content of M₁ was 20 wt% and 30 wt% in the E_V-PDLC film cured by TTMP, the sample microscopically formed dense and uniform layered structures, and the thermal conductivity reached 0.75 W m^-1 K^-1. In the PETMP curing system, when the content of M₁ was 20 wt%, the sample microscopically formed compact spherical ordered structures, and the thermal conductivity increased to 0.78 W m^-1 K^-1. When the content of M₁ was 30 wt%, the microscopic order of the E_V-PDLC film was destroyed, and the thermal conductivity decreased sharply to 0.64 W m^-1 K^-1. The applied electric field promoted the orderly orientation of M₁ and epoxy molecular chains, maked the ordered structure in the E_V-PDLC film more uniform and dense, to the benefit of stabilizing well on the orderly arrangement of liquid crystal molecules.

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