Polymer ( IF 4.1 ) Pub Date : 2018-10-17 , DOI: 10.1016/j.polymer.2018.10.035 Ihor Tkachenko , Yuriy Kononevich , Yaroslav Kobzar , Olha Purikova , Yurii Yakovlev , Ivan Khalakhan , Aziz Muzafarov , Valery Shevchenko
In this work, for the first time, we describe the design and synthesis of novel fluorinated poly(arylene ether)/silica cross-linked materials (FPAE/SiO1.5) through a sol-gel process by using the triethoxysilyl-containing fluorinated polyethers as precursors for both organic and inorganic networks formation. The polyether-based precursors with the sol-gel active species were synthesized via hydrosilylation reaction between triethoxysilane and the corresponding allyl-functionalized FPAE under Pt catalysis. Herein, we present two approaches of hydrolysis triethoxysilane groups to silanol ones within sol-gel chemistry: (1) hydrolysis with air moisture and (2) hydrolysis of the ethoxysilyl groups at the interface between two liquids. The mechanical and thermal properties of the FPAE/SiO1.5 materials were studied depending on the structure of macromolecular chains and synthetic route. Scanning electron and atomic force microscopies were employed to investigate the morphology of the resulting silica-containing cross-linked materials. The resulting FPAE/SiO1.5 films were flexible and tough with tensile strength above 25 МPа, and exhibited high thermal stability, having the initial decomposition temperature about 300°С. For more detailed explanation of the thermophysical behavior of the FPAE/SiO1.5 materials, the synthesis method of new silica-containing organic-inorganic system was developed by the direct hydrosilylation reaction between allyl-functionalized polyethers and 1,1,3,3-tetramethyldisiloxane. All films exhibited high hydrophobic properties (water contact angles above 102°), low dielectric constants and losses at room temperature. In particular, the FPAE/SiO1.5 film prepared from tetrafluorobenzene-based polyether showed the ultra-low dielectric constant of 1.86 at 10 kHz. This makes the obtained polymer FPAE/SiO1.5 materials attractive for microelectronics and many other emerging applications.
中文翻译:
基于氟化聚亚芳基醚的低介电常数含二氧化硅的交联有机-无机材料
在这项工作中,我们首次描述了使用含三乙氧基甲硅烷基的氟化聚醚作为溶胶-凝胶工艺,设计和合成新型氟化聚(亚芳基醚)/二氧化硅交联材料(FPAE / SiO 1.5)。有机和无机网络形成的前体。在Pt催化下,通过三乙氧基硅烷与相应的烯丙基官能化的FPAE之间的硅氢加成反应,合成了具有溶胶-凝胶活性物种的基于聚醚的前体。在本文中,我们提出了在溶胶-凝胶化学中将三乙氧基硅烷基团水解为硅烷醇的两种方法:(1)用空气湿气水解和(2)两种液体之间的界面处的乙氧基硅烷基团的水解。FPAE / SiO 1.5的机械和热性能根据高分子链的结构和合成途径对材料进行了研究。使用扫描电子和原子力显微镜检查所得到的含二氧化硅的交联材料的形态。所得的FPAE / SiO 1.5薄膜具有柔韧性和韧性,拉伸强度高于25МPа,并显示出高的热稳定性,其初始分解温度约为300°C。有关FPAE / SiO 1.5的热物理行为的更详细说明通过烯丙基官能化聚醚与1,1,3,3-四甲基二硅氧烷的直接硅氢化反应,开发了新型的含二氧化硅有机-无机体系的合成方法。所有薄膜均表现出高疏水性(水接触角大于102°),低介电常数和在室温下的损耗。特别地,由基于四氟苯的聚醚制备的FPAE / SiO 1.5膜在10kHz处显示出1.86的超低介电常数。这使得获得的聚合物FPAE / SiO 1.5材料对微电子学和许多其他新兴应用具有吸引力。