引用本文:吴连锋,朱洪宇,申小松,朱艳吉,汪怀远.1,5-萘二酚改性环氧树脂及其氮化硼复合材料的制备与导热性能[J].中国表面工程,2024,37(1):110~117
WU Lianfeng,ZHU Hongyu,SHEN Xiaosong,ZHU Yanji,WANG Huaiyuan.Preparation and Thermal Conductivity of 1, 5-Naphthalenediol Modified Epoxy Resin and Boron Ntride Composite[J].China Surface Engineering,2024,37(1):110~117
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1,5-萘二酚改性环氧树脂及其氮化硼复合材料的制备与导热性能
吴连锋1, 朱洪宇2, 申小松2, 朱艳吉2, 汪怀远3
1.海洋化工研究院有限公司海洋涂料国家重点实验室 青岛 266071;2.天津大学材料科学与工程学院 天津 300350;3.天津大学化工学院 天津 300350
摘要:
环氧树脂是导热复合材料领域必不可少的,但是由于其本征导热系数较低限制了应用,因此提高环氧树脂本征导热系数对于高性能导热复合材料的开发具有重要意义。环氧树脂本征热导率的提高通常可采用引入刚性基团的方式实现,而实际操作中往往受限于含刚性基团分子与环氧树脂分子之间存在极性差异、相容性不一致等问题,导致环氧树脂及其复合材料结构设计与合成具有复杂性,限制了其实际应用。采用含较强刚性萘环的 1, 5-萘二酚(Naphthalenediol)改性环氧树脂(EP) 制备萘改性环氧树脂(NEP),改善环氧树脂分子链的“有序性”,减少导热过程中声子的散射,提高材料的导热性。研究结果表明,NEP 的导热系数为 0.32 W / (m·K),是 EP 导热系数 0.19 W / (m·K)的 1.68 倍。氮化硼(BN)填料的加入使 NEP / BN 复合材料的热导率提升至 1.25 W / (m·K),为 EP / BN 复合材料热导率 1.01 W / (m·K)的 1.24 倍,EP 的 6.58 倍。NEP 及 NEP / BN 复合材料导热性能的提升,归因于萘环的刚性引起分子链的排列更加有序,以及改性过程中形成氢键的协同作用。 向环氧树脂中引入萘环结构,采用简单的试验操作,明显提高了环氧树脂的本征热导率,可以为具有良好导热性能的树脂材料的开发提供思路。
关键词:  环氧树脂  1  5-萘二酚  导热  改性  热导率
DOI:10.11933/j.issn.1007-9289.20230223001
分类号:TB332
基金项目:国家自然科学基金(21676052,21606042);国家自然科学基金杰出青年基金(51925403);海洋涂料国家重点实验室开放课题基金
Preparation and Thermal Conductivity of 1, 5-Naphthalenediol Modified Epoxy Resin and Boron Ntride Composite
WU Lianfeng1, ZHU Hongyu2, SHEN Xiaosong2, ZHU Yanji2, WANG Huaiyuan3
1.State Key Laboratory of Marine Coatings, Marine Chemical Research Institute Co., Ltd.,Qingdao 266071 , China;2.School of Materials Science and Engineering, Tianjin University, Tianjin 300350 , China;3.School of Chemical Engineering, Tianjin University, Tianjin 300350 , China
Abstract:
Polymer-based composite materials are widely used in the field of thermal conductivity owing to their low weight, electrical insulation, heat resistance, corrosion resistance, and excellent mechanical properties. Epoxy resin (EP) is essential in the field of thermally conductive composite materials; however, its low intrinsic thermal conductivity limits its application. Therefore, improving the intrinsic thermal conductivity of EP is crucial for developing high-performance thermally conductive composite materials. An improvement in the thermal conductivity of EP composite materials can be achieved by increasing the content of inorganic fillers; however, excessive inorganic fillers also affect the processing performance of the composite materials. Therefore, improving the intrinsic thermal conductivity of EP is important. Generally, the intrinsic thermal conductivity of EP can be improved by introducing molecules with rigid groups. However, in practical operations, limitations often exist, such as polarity differences and inconsistent compatibility between molecules containing rigid groups and EP molecules, which result in complexity in the structural design and synthesis of EP and its composite materials, limiting their practical applications. In this paper, the naphthalenediolmodified EP (NEP) was prepared by the reaction of the strong rigidity naphthalenediol and EP, aiming to improve the "order" of the EP molecular chain. When naphthalene glycol is used as a thermally conductive material, the rigid groups of naphthalene glycol reduce phonon scattering and improve the thermal conductivity of NEP and the corresponding composite materials with thermally conductive fillers. When used as a thermally conductive material, the rigid groups of naphthalenediol reduce the scattering of phonons and improve the thermal conductivity of NEP and the corresponding composites incorporating thermally conductive fillers. Infrared analysis indicated that the 1,5-naphthalene diphenol-modified EP consumed some epoxy groups, indicating the occurrence of a NEP modification reaction. The thermal conductivity of NEP was 0.32 W / (m·K), which was 1.68 times that of EP (0.19 W / (m·K)). To determine the effect of the 1,5-naphthalene diphenol content on the thermal conductivity of the NEP and NEP / BN composite materials, we conducted tests on the thermal conductivity of the materials at different mass ratios and curing temperatures. The increase rate of the thermal conductivity of the NEP / BN composite material was always greater than that of EP / BN composite material. Specifically, after adding BN filler with a weight ratio of 30%, the thermal conductivity of the NEP / BN composite increased to 1.25 W / (m·K), which was 1.24 times that of EP / BN composite (1.01 W / (m·K)) and 6.58 times that of EP. The increase in the NEP and EP / BN composite materials is primarily because the EP modified with a rigid naphthalene ring is more likely to form a thermal conductivity network within the molecule, improving the thermal conductivity of the composite material. Furthermore, the infrared thermal imager recorded the changes in surface color and temperature of the EP (a1), NEP (a2), EP / BN (a3), and NEP / BN (a4) composite materials over time. After BN was added, the surface color change of the NEP / BN and EP / BN composite materials was significantly faster than that of NEP and EP, and the surface temperature change of all samples became more pronounced with increasing heating time. The mechanism analysis showed that after NEP was heated, phonons were transmitted along the EP naphthalene molecular chain. Because of the relatively complete planar structure of the naphthalene ring, the phonons transmitted here were efficiently transmitted on its surface, reducing the probability of phonon scattering and thereby improving thermal conductivity. This study provides insights into improving the thermal conductivities of modified EP and its composite materials.
Key words:  epoxy resin  naphthalenediol  thermal conduction  modification  thermal conductivity
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