氮化硼/聚合物导热复合材料界面热阻调控研究进展

doi:10.11896/cldb.21080118

材料导报

2023, Vol. 37

Issue (18): 21080118-13 https://doi.org/10.11896/cldb.21080118

高分子与聚合物基复合材料

氮化硼/聚合物导热复合材料界面热阻调控研究进展

张荣^*, 刘卓航, 熊文伟, 林乾辉, 何学航, 李思琦, 刘清亭, 付旭东, 胡圣飞

湖北工业大学绿色轻工材料湖北省重点实验室,武汉 430068

Recent Progress of Interface Thermal Resistance Regulation of Thermally Conductive Composites Based on Boron Nitride/Polymer

ZHANG Rong^*, LIU Zhuohang, XIONG Wenwei, LIN Qianhui, HE Xuehang, LI Siqi, LIU Qingting, FU Xudong, HU Shengfei

Hubei Provincial Key Laboratory of Green Materials for Light Industry, Hubei University of Technology, Wuhan 430068, China

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摘要随着5G时代的发展,电子器件领域的热管理问题日发严峻。氮化硼(BN)是一类高热导率(TC)、高绝缘的导热填料,广泛应用于热管理领域,包括六方氮化硼(h-BN)、氮化硼纳米片(BNNS)和氮化硼纳米管(BNNT)。然而,BN表面呈化学惰性,其与基体或其他填料间亲和力低、声子谱失配等,导致了填料与基体/填料间存在明显的界面热阻,限制了复合材料TC的提升,难以满足使用要求。因此,如何调控界面热阻、设计BN/聚合物导热复合材料的热传导界面,并提高复合材料的导热能力是当前亟待解决的难题。
研究者分别从理论模拟与实验验证两个角度对热流在界面传导的差异及其原因进行探索。在理论研究中,将分子动力学(MD)模拟及有限元模拟(FEA)等方法结合有效介质模型及其优化模型、Foygel模型等能够对界面热阻(ITR)进行深入的理论模拟与分析;其中,影响界面热阻的关键参数包括BN含量、尺寸及晶体状态、BN的分布形貌等。在实验设计中,为了改善填料与基体间界面热阻,首先对BN表面共价键改性或表面包覆,随后结合聚合物种类设计相应的官能团来改善BN与聚合物的界面作用力;其中BN表面的共价键改性对BN本身晶体结构有一定的破坏,表面包覆则能够较好地保持BN结构。为了改善填料与填料间界面热阻,研究者常采用BN的定向排列、桥接、构建3D导热网络结构等策略来改善填料间的接触,其中BN的定向排列法充分利用BN的各向异性、增大填料间的有效接触面积,能够显著提升复合材料某一方向的TC;桥接法是将彼此分离的BN相互连接,通过在基体中形成异质结构来构建更为完善的导热路径;构建3D导热网络结构的方法近年来已被广泛研究,其能够创建长程连续的导热路径,具体方法包括冰模板法、盐模板、发泡策略、构建凝胶网络和两相/三相隔离结构等。
综合目前研究进展,本文首先归纳了计算BN/聚合物界面热阻的模型及相关模拟的进展,并从填料与基体及填料与填料间的界面热阻两个角度,分别总结了改善聚合物/BN导热复合材料界面热阻的策略,对比了各种方法对复合材料导热性能的改善效果,并展望了低界面热阻与高导热复合材料的发展趋势。

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	张荣
	刘卓航
	熊文伟
	林乾辉
	何学航
	李思琦
	刘清亭
	付旭东
	胡圣飞

关键词: 导热复合材料氮化硼(BN) 聚合物填料与基体间界面热阻(ITR_F-M) 填料与填料间界面热阻(ITR_F-F)

Abstract: With the development of 5G communication, thermal management has become an increasingly severe problem in electronic devices. Boron nitride (BN) is a category of high-thermal-conductivity (TC) and highly insulating thermally conductive fillers widely used in thermal management, including hexagonal boron nitride (h-BN), boron nitride nanosheets (BNNSs), and boron nitride nanotubes (BNNTs). However, the BN surface is chemically inert, and its low affinity and phonon-spectrum mismatch with the matrix or other fillers lead to significant interfacial thermal resistance (ITR) between the filler and matrix/filler, which limits the enhancement of TC of the composites and makes it difficult to meet usage requirements. Therefore, how to regulate the ITR, design the thermal conductivity interface of BN/polymer thermally conductive composites, and improve the thermal conductivity of the composites is a current challenge.
Researchers have explored the differences and causes of heat-flow conduction at the interface from two separate perspectives: theoretical simulation and experimental verification. In theoretical studies, molecular dynamics (MD) simulations and finite element analysis (FEA) methods combined with models such as effective medium model and its optimization model, Foygel model, are used for in-depth theoretical simulation and analysis of ITR. Among these, the key parameters affecting ITR include BN content, size and crystal state, and BN distribution morphology, among others. In experimental design, to improve the ITR between the filler and substrate, the BN surface is first modified by covalent bonding or surface coating, and then the corresponding functional groups are designed to improve the interfacial force with the polymer in combination with the polymer species. Among these, the covalent bonding modification of the BN surface causes some damage to the BN crystal structure itself, while surface coating can better maintain the BN structure. To improve the ITR between fillers, researchers often use strategies such as BN orientation arrangement, bridging, and construction of three-dimensional (3D) thermal network structure to improve the contact between fillers. The bridging method is used to connect the separated BN to each other to build better thermal conductivity paths by forming heterogeneous structures in the matrix. Methods of building 3D thermal network structures that can create long-range continuous thermal conductivity paths have been widely developed in recent years and include the ice template method, salt templates, the foaming strategy, building a gel network, and two-phase/three-phase isolated structure.
The current level of research progress is summarized in this review. First, we summarize the models used to calculate the thermal resistance of the BN/polymer interface and the progress of related simulations, and summarize the strategies for optimizing ITR of polymer/BN thermally conductive composites from two separate perspectives, i.e., those of ITR between the filler and matrix/filler. In addition, we compare the effect of various methods on improving the TC of composites and look forward to the development trend of low-ITR and high-TC composites.

Key words: thermally conductive composites boron nitride (BN) polymer interfacial thermal resistance between filler and matrix (ITR_F-M) interfacial thermal resistance between filler and filler (ITR_F-F)

出版日期: 2023-09-25 发布日期: 2023-09-18

ZTFLH:

TB332

基金资助: 国家自然科学基金(51503061);湖北省自然科学基金(2015CFB322;2015BAA094);武汉市知识创新专项(2022010801020261)

通讯作者: *张荣,湖北工业大学教授。主要研究领域为聚合物基导电、导热功能复合材料及聚合物材料的改性与加工。目前主持国家自然科学基金项目1项,主持完成省部级项目2项,企业合作项目4项。发表学术论文65余篇,以第一或通信作者发表30篇,其中SCI、EI论文29篇。获国家发明专利8项。zhangrong@hbut.edu.cn

引用本文:

张荣, 刘卓航, 熊文伟, 林乾辉, 何学航, 李思琦, 刘清亭, 付旭东, 胡圣飞. 氮化硼/聚合物导热复合材料界面热阻调控研究进展[J]. 材料导报, 2023, 37(18): 21080118-13.
ZHANG Rong, LIU Zhuohang, XIONG Wenwei, LIN Qianhui, HE Xuehang, LI Siqi, LIU Qingting, FU Xudong, HU Shengfei. Recent Progress of Interface Thermal Resistance Regulation of Thermally Conductive Composites Based on Boron Nitride/Polymer. Materials Reports, 2023, 37(18): 21080118-13.

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http://www.mater-rep.com/CN/10.11896/cldb.21080118 或 http://www.mater-rep.com/CN/Y2023/V37/I18/21080118

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