Mukun He#, Lei Zhang#, Kunpeng Ruan, Junliang Zhang, Haitian Zhang, Peng Lv, Yongqiang Guo, Xuetao Shi, Hua Guo*, Jie Kong and Junwei Gu*. Functionalized Aluminum Nitride for Improving Hydrolysis Resistances of Highly Thermally Conductive Polysiloxane Composites. Nano-Micro Letters, 2025, 17: 134. 2023IF=31.6.（1区材料科学Top期刊）
https://doi.org/10.1007/s40820-025-01669-5
Abstract
A series of divinylphenyl-acryloyl chloride copolymers (PDVB-co-PACl) is synthesized via atom transfer radical polymerization employing tert-butyl acrylate and divinylbenzene as monomers. PDVB-co-PACl is utilized to graft on the surface of spherical aluminum nitride (AlN) to prepare functionalized AlN (AlN@PDVB-co-PACl). Polymethylhydrosiloxane (PMHS) is then used as the matrix to prepare thermally conductive AlN@PDVB-co-PACl/PMHS composites with AlN@PDVB-co-PACl as fillers through blending and curing. The grafting of PDVB-co-PACl synchronously enhances the hydrolysis resistance of AlN and its interfacial compatibility with PMHS matrix. When the molecular weight of PDVB-co-PACl is 5100 g/mol and the grafting density is 0.8 wt%, the compositescontaining 75 wt% of AlN@PDVB-co-PACl exhibit the optimal comprehensive performance. The thermal conductivity (λ) of the composite is 1.14 W/(m·K), which enhances by 20% and 420% compared to the λ of simply physically blended AlN/PMHS composite and pure PMHS, respectively. Meanwhile, AlN@PDVB-co-PACl/PMHS composites display remarkable hydrothermal aging resistance by retaining 99.1% of its λ after soaking in 90℃ deionized water for 80 hours, whereas the λ of the blended AlN/PMHS composites decreases sharply to 93.7%.
本研究以丙烯酸叔丁酯为单体和二乙烯基苯为支化单元，通过原子转移自由基聚合合成具有支化结构的二乙烯基苯-丙烯酰氯无规共聚物（PDVB-co-PACl）。以聚甲基氢硅氧烷（PMHS）为基体、PDVB-co-PACl表面接枝改性的AlN（AlN@PDVB-co-PACl）为导热填料，经共混复合-热固化制备AlN@PDVB-co-PACl/PMHS导热复合材料。无规共聚物的成功接枝同步提升了AlN的耐水解性能及其与PMHS基体间的界面相容性。当PDVB-co-PACl分子量为5100 g/mol、AlN@PDVB-co-PACl的质量分数为75 wt%且其表面PDVB-co-PACl接枝量为0.8 wt%时，AlN@PDVB-co-PACl/PMHS导热复合材料具有最优的综合性能，其λ为1.14 W/(m·K)，较简单共混AlN/PMHS和纯PMHS的λ分别提升了20%和420%，且在90℃去离子水中浸泡80小时后的λ保持率为99.1%，明显优于AlN/PMHS导热复合材料同样处理后的λ保持率（93.7%）。
论文亮点
1. 设计合成了提升AlN耐水解性的具有支化结构的二乙烯基苯-丙烯酰氯无规共聚物（PDVB-co-PACl）。
2. 优化PDVB-co-PACl分子量为5100 g/mol时，其具有最佳的耐水解性、最低的界面热阻。
3. 当AlN@PDVB-co-PACl的质量分数为75 wt%且其表面PDVB-co-PACl接枝量为0.8 wt%时，AlN@PDVB-co-PACl/PMHS复合材料的λ为1.14 W/(m·K)，在90℃去离子水中浸泡80小时后λ保持率为99.1%。
第一作者：何沐锟、张磊
邮件地址：hemukun@mail.nwpu.edu.cn、18695349879@163.com
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