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

大分子单体 材料科学 电介质 硅氢加成 玻璃化转变 透射率 倍半硅氧烷 高分子化学 耗散因子 介电常数 聚合物 热稳定性 介电损耗 复合材料 化学工程 催化作用 有机化学 化学 光电子学 共聚物 工程类
作者
Jiajia Wang,Junfeng Zhou,Kaikai Jin,Liang Wang,Jing Sun,Qiang Fang
出处
期刊:Macromolecules [American Chemical Society]
卷期号:50 (23): 9394-9402 被引量:95
标识
DOI:10.1021/acs.macromol.7b02000
摘要

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 (Dk) of 2.50 and low dissipation factor (Df) of 4.0 × 10–3 at an ultrahigh frequency of 10 GHz. This is the first example of nonporous polysiloxane having both low Dk and Df while conventional TEOS-based polymers exhibit higher Dk (>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 (Tg) 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 Tg 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 Dk and Df.
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