低介电耐温改性空心SiO_(2)填充含氟聚芳醚腈复合材料的制备及性能

Preparation and properties of low dielectric and temperature-resistant poly(aryl ether nitrile)composites filled with modified hollow SiO_(2)

开发低介电常数、低介电损耗和同时兼具耐温、高力学强度的聚合物介电材料对于满足5G领域的高性能介电材料具有重要的研究意义。采用含氟1H,1H,2H,2H-全氟取代癸基三乙氧基硅烷(PTES)对空心SiO_(2)纳米粒子(HS)进行表面改性,并基于含氟聚芳醚腈共聚物(PEN-F),分别以流延法和相转换法制备了两种PTES改性HS填充的PEN-F复合材料(HS@PTES/PEN-F)。采用FTIR和1H NMR证实了PEN-F共聚物的成功合成;通过FTIR、TGA和XPS等技术手段表征了PTES改性的HS结构和形貌;同时研究了HS@PTES/PEN-F复合材料的介电性能、力学强度和热稳定性等。研究结果表明,经PTES改性后的HS纳米粒子在PEN-F基体树脂中具有较好的分散性与界面相容性。在介电性能方面,当改性SiO_(2)纳米粒子填充含量为7wt%时,通过流延法制备的HS@PTES/PEN-F复合膜在1 kHz时介电常数达2.88,介电损耗为0.0198;通过相转换法制备的HS@PTES/PEN-F复合膜在1 kHz时介电常数达1.19,介电损耗为0.0043。在力学性能方面,以相转换法为例,改性SiO_(2)纳米粒子填充含量为5wt%时,其拉伸强度和弹性模量分别达到10.34 MPa和365.32 MPa。此外,HS@PTES/PEN-F复合膜的玻璃化转变温度可达到160℃,具有较好的热稳定性。

The development of polymer dielectric materials with low dielectric constant,low dielectric loss,temperature resistance and high mechanical strength is of great significance to meet the requirements of high performance dielectric materials in 5G field.The hollow SiO_(2) nanoparticles(HS)were modified by 1H,2H,2H-perfluorooctyltriethoxysilane(PTES),and two kinds of low dielectric poly(aryl ether nitrile)composites(HS@PTES/PEN-F)were prepared by solution casting and phase conversion methods based on fluorinated poly(aryl ether nitrile)copolymer(PEN-F).The successful synthesis of fluorinated poly(aryl ether nitrile)copolymer was confirmed by FTIR and 1H NMR;the structure and morphology of PTES modified HS were characterized by FTIR,TGA and XPS.At the same time,the dielectric properties,mechanical strength and thermal stability of the HS@PTES/PEN-F composites were studied.The results show that the HS modified by PTES exhibit good dispersion and interface compatibility in the PEN-F matrix resin.In terms of dielectric properties,when the content of modified SiO_(2) nanoparticles reaches 7wt%,the dielectric constant and the dielectric loss of the HS@PTES/PEN-F composite film prepared by solution casting method are 2.88 and 0.0198 at 1 kHz;the dielectric constant and dielectric loss of the HS@PTES/PEN-F composite film prepared by phase conversion method are 1.19 and 0.0043,respectively.In the aspect of mechanical properties,taking the phase conversion method as an example,when the content of modified SiO_(2) nanoparticles reaches 5wt%,the tensile strength and elasticity modulus increase to 10.34 MPa and 365.32 MPa,respectively.In addition,the glass transition temperature of HS@PTES/PEN-F composite film can reach 160℃,which shows good thermal stability.