Functionalized Aluminum Nitride for Improving Hydrolysis Resistances of Highly Thermally Conductive Polysiloxane Composites

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⁻¹ and the grafting density is 0.8 wt%, the composites containing 75 wt% of AlN@PDVB-co-PACl exhibit the optimal comprehensive performance. The thermal conductivity (λ) of the composite is 1.14 W m⁻¹ K⁻¹, 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 °C deionized water for 80 h, whereas the λ of the blended AlN/PMHS composites decreases sharply to 93.7%. (Figure presented.)