Mechanism and Performance of Asymmetric Triazine Networks Formed in Cyanate Ester Resins Induced by Polysilazane

The rapid advancement of high-frequency communications, aerospace, and electronic packaging demands high-performance resin matrices. Cyanate ester (CE) resins are promising matrices due to their high strength, excellent dielectric properties, and thermal stability, but their long polymerization process and inherent brittleness hinder broader application. In this study, we introduced poly(dimethylsilazane) (MPSZ) containing reactive amine groups into a bisphenol A dicyanate (BADCy) system. This approach effectively lowers the curing activation energy and reduces the peak curing temperature by as much as 116 °C, all while preserving a favorable processing window and room-temperature storage stability. Acting simultaneously as a catalyst and a network modifier, MPSZ promotes the construction of an organic–inorganic hybrid network. Mechanistic investigations reveal a chain-growth insertion pathway induced by MPSZ, wherein flexible silazane segments are covalently incorporated into the cross-linked framework via the formation of asymmetric triazine structures, thereby enabling effective regulation of the network structure. The cured hybrid network exhibits simultaneously enhanced properties, with the dielectric constant at 1 MHz dropping to 2.68 with a loss tangent of 0.0026, moisture absorption decreasing by 36%, and impact strength reaching 35.08 kJ/m 2 . Collectively, this work provides a theoretical and experimental foundation for the design of high-performance CE matrices that cured at low temperatures, offering considerable potential for advanced electronic and aerospace applications.