A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS),Macromolecules

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A New Fluorinated Polysiloxane with Good Optical Properties and Low Dielectric Constant at High Frequency Based on Easily Available Tetraethoxysilane (TEOS)
Macromolecules ( IF 5.1 ) Pub Date : 2017-11-21 00:00:00 , DOI: 10.1021/acs.macromol.7b02000
Jiajia Wang ₁ , Junfeng Zhou ₁ , Kaikai Jin ₁ , Liang Wang ₂ , Jing Sun ₁ , Qiang Fang ₁

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A novel fluorinated macromonomer (TFVE-Si) with four functional groups derived from easily available tetraethoxysilane (TEOS) has been successfully synthesized through the Piers–Rubinsztajn reaction using B(C₆F₅)₃ as a catalyst. This procedure efficiently avoids the generation of Si–OH and −Si–CH₂–CH₂– groups, which greatly affect the properties of the organosiloxanes. Prepolymerizing the macromonomer in mesitylene solution gives an oligomer which can form a flexible and highly transparent free-standing cross-linked polysiloxane film followed by a postpolymerization procedure at high temperature. The cross-linked polysiloxane (thickness = 2 mm) shows a transmittance of higher than 91% in the visible region and an absorbance of near 100% in the UV region (<350 nm), exhibiting its potential application as a transparent coating for blocking ultraviolet rays in both household and industrial uses. In particular, the cross-linked film shows low dielectric constant (D_k) of 2.50 and low dissipation factor (D_f) of 4.0 × 10^–3 at an ultrahigh frequency of 10 GHz. This is the first example of nonporous polysiloxane having both low D_k and D_f while conventional TEOS-based polymers exhibit higher D_k (>3.0). Moreover, D–E loop tests illustrate that the cross-linked polysiloxane possesses excellent linear dielectric properties, further suggesting its good insulating properties. Furthermore, the prepared polysiloxane exhibits high thermostability with a 5 wt % loss temperature of 476 °C and a glass transition temperature (T_g) of 110 °C as well as good mechanical strength (with an elastic modulus of 1.1 GPa). Because of the existence of fluoro-containing groups, the polysiloxane also shows high hydrophobicity. Furthermore, TFVE-Si can efficiently improve the T_g of linear polysiloxane prepared from dimethylsiloxane with two functional groups. These indicate that the fluorinated TEOS has potential application in the microelectronics industry; especially, it can meet the requirement of the high-frequency communication fields for the materials with both low D_k and D_f.

中文翻译：

基于易于获得的四乙氧基硅烷（TEOS）的一种新型的，具有良好的光学性能和较低的高频介电常数的氟化聚硅氧烷

通过使用B（C ₆ F ₅）₃作为催化剂，通过Piers-Rubinsztajn反应成功地合成了具有四个官能团的新型氟化大分子单体（TFVE-Si），该官能团衍生自易于获得的四乙氧基硅烷（TEOS）。此过程有效地避免了Si-OH和-Si-CH ₂ -CH _2的产生–会极大影响有机硅氧烷性能的基团。在均三甲苯溶液中预聚合大分子单体可形成低聚物，该低聚物可形成柔性且高度透明的自立式交联聚硅氧烷薄膜，随后在高温下进行后聚合步骤。交联的聚硅氧烷（厚度= 2毫米）在可见光区域的透射率高于91％，在紫外光区域（<350 nm）的吸收率接近100％，显示出其潜在的用途，可作为用于粘连的透明涂层家用和工业用紫外线。尤其是，该交联膜显示出2.50的低介电常数（D _k）和4.0×10 ^–3的低耗散系数（D _f）。在10 GHz的超高频率下。这是具有低D _k和D _f的无孔聚硅氧烷的第一个例子，而常规的基于TEOS的聚合物表现出较高的D _k（> 3.0）。此外，D – E回路测试表明，交联的聚硅氧烷具有出色的线性介电性能，进一步表明了其良好的绝缘性能。此外，制得的聚硅氧烷表现出高的热稳定性，损失温度为5 wt％，为476°C，玻璃化转变温度为（T _g）以及110℃的良好机械强度（具有1.1 GPa的弹性模量）。由于存在含氟基团，聚硅氧烷也显示出高疏水性。此外，TFVE-Si可以有效地改善由具有两个官能团的二甲基硅氧烷制得的线性聚硅氧烷的T _g。这些表明氟化的TEOS在微电子工业中具有潜在的应用。特别是，对于D _k和D _f都低的材料，可以满足高频通信领域的要求。

更新日期：2017-11-21

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