同时改善具有甲硅烷基醚侧基的芴基聚酰亚胺的光学、介电和溶解性能,ACS Omega

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同时改善具有甲硅烷基醚侧基的芴基聚酰亚胺的光学、介电和溶解性能
ACS Omega ( IF 3.7 ) Pub Date : 2022-04-01 , DOI: 10.1021/acsomega.2c00069
Yancheng Wu _{1,

2} , Shumei Liu ₂ , Jianqing Zhao ₂

Affiliation

通过含羟基聚酰亚胺 (OH-PIs) 和叔丁基氯二苯基硅烷 (TBDPSCl)的简单高效的硅醚化反应，成功合成了三种具有硅醚基团的芴基聚酰亚胺 (Si-PIs) ，其结构由¹ H NMR和IR光谱。笨重的非极性叔叔改性PI单元中的-丁基二苯基甲硅烷基（TBDPS）侧基而不是强电子供体-OH基团有利于减少沿PI链的电子共轭和电荷转移（CT）相互作用。因此，与前驱体 OH-PI 薄膜相比，改性 Si-PI 薄膜的光学、介电和溶解度性能同时得到改善。改性的 Si-PI 薄膜在 400 nm ( T ₄₀₀) 从 42% 到 55% 的 OH-PI 薄膜从 74% 到 81% 以及荧光特性的再生。由于被大体积的非极性 TBDPS 基团取代，Si-PI 薄膜的介电常数和损耗在 1 kHz 时也明显从 OH-PI 薄膜的 4.19 到 4.78 和 0.0173-0.0295 分别降低到 2.63-2.75 和 0.0024-0.0091增加Si-PI薄膜的自由体积和疏水性。Si-PIs 在低极性或非极性溶剂（如 CHCl ₃、CH ₂ Cl ₂、丙酮和甲苯）中的溶解度显着提高。此外，Si-PI 薄膜仍保持较好的热性能，在氮气氛下的 5% 失重温度 ( T _5% ) 在 470-491 °C 范围内和玻璃化转变温度 (T _g ) 在 245–308 °C 范围内。

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Simultaneously Improving the Optical, Dielectric, and Solubility Properties of Fluorene-Based Polyimide with Silyl Ether Side Groups

Three fluorene-based polyimides with silyl ether groups (Si–PIs) were successfully synthesized by a simple and efficient silicon etherification reaction of hydroxyl-containing polyimides (OH–PIs) and tert-butylchlorodiphenylsilane (TBDPSCl), and their structures were confirmed by ¹H NMR and IR spectra. The bulky nonpolar tert-butyldiphenylsilyl (TBDPS) side groups in the modified PI unit instead of the strong electron donor −OH group is conducive to decreasing electronic conjugation and charge transfer (CT) interaction along the PI chain. Accordingly, the optical, dielectric, and solubility properties of the modified Si–PI films are simultaneously improved compared with the precursor OH–PI films. The modified Si–PI films demonstrate a meaningful enhancement in the transmittances at a wavelength of 400 nm (T₄₀₀) to 74–81% from 42 to 55% of OH–PI films and the regeneration of fluorescence characteristics. The dielectric constant and loss of Si–PI films are also obviously reduced to 2.63–2.75 and 0.0024–0.0091 at 1 kHz from 4.19 to 4.78 and 0.0173–0.0295 of OH–PI films, respectively, due to substituted with the bulky nonpolar TBDPS groups to increase the free volume and hydrophobicity of Si–PI films. The solubility of Si–PIs in low- or nonpolar solvents (such as CHCl₃, CH₂Cl₂, acetone, and toluene) is significantly improved. Furthermore, Si–PI films still maintain relatively good thermal properties with the 5% weight loss temperature (T_5%) in the range 470–491 °C under a nitrogen atmosphere and the glass transition temperature (T_g) in the range 245–308 °C.

更新日期：2022-04-01

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