具有保持绝缘和热性能的本征黑色聚酰亚胺：一种能够线性共聚的黑色蒽醌衍生物,Macromolecules

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具有保持绝缘和热性能的本征黑色聚酰亚胺：一种能够线性共聚的黑色蒽醌衍生物
Macromolecules ( IF 5.1 ) Pub Date : 2021-10-08 , DOI: 10.1021/acs.macromol.1c01422
Yu Zhou ₁ , Songyang Zhang ₁ , Feng Zheng ₁ , Qinghua Lu _{1,

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Affiliation

黑色聚酰亚胺（BPI）代替黄色透明聚酰亚胺在光电器件的发展中的需求越来越大，但掺杂炭黑的BPI由于针孔和分散不均匀而表现出严重的绝缘和机械性能缺陷。因此，本质上 BPI 已经引起了科学和工业界越来越多的兴趣。蒽醌衍生物具有足够高的摩尔消光系数 (ε)，并附加了尽可能多的辅助色素（-OH 和 -NH ₂) 尽可能在蒽醌骨架上扩展其光吸收范围，从而实现完全的紫外-可见光吸收。然而，其在 BPI 中应用的最大障碍是保留单体双功能性以避免凝胶形成。在这项工作中，开发了一种可线性聚合的蒽醌衍生物，2,4,5,7-tetraamino-1,8-dihydroxyanthracene-9,10-dione (4NADA)。这种带有多个活性基团的单体的结构分析¹H NMR、傅里叶变换红外和理论计算表明，由于分子内氢键的形成，辅助色素基团表现出不同的亲核活性，因此只有对氨基（2-和7-位）可以参与聚合反应。随后，4NADA 共聚成 Kapton 型聚酰亚胺。我们发现，4NADA (4%) 的低水平引入提供了一种光谱 BPI 薄膜，该薄膜保持了聚酰亚胺的电绝缘和耐热性能。该方法相当于在聚酰亚胺链中嵌入黑色单体，具有经济性、通用性、工艺一致性、易于访问和性能优越等优点。

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Intrinsically Black Polyimide with Retained Insulation and Thermal Properties: A Black Anthraquinone Derivative Capable of Linear Copolymerization

Black polyimide (BPI) is increasingly in demand for the development of photoelectric devices in place of yellow transparent polyimide, but BPI doped with carbon black shows serious insulation and mechanical performance deficiencies due to pinholes and uneven dispersion. Intrinsically BPI has thus attracted increasing interest in science and industry. Anthraquinone derivatives have an ample high molar extinction coefficient (ε), and appending as many auxochromes (−OH and −NH₂) as possible on the anthraquinone skeleton can extend its light absorption range, thereby achieving complete UV–visible light absorption. However, the greatest obstacle to its application in BPI is retaining the monomer bifunctionality to avoid gel formation. In this work, a linearly polymerizable anthraquinone derivative, 2,4,5,7-tetraamino-1,8-dihydroxyanthracene-9,10-dione (4NADA), has been developed. Structural analysis of this monomer bearing multiple active groups by ¹H NMR, Fourier-transform infrared, and theoretical calculations has demonstrated that the auxochrome groups show different nucleophilic activities owing to the formation of intramolecular hydrogen bonds, such that only p-amino groups (2- and 7-positions) can participate in the polymerization reaction. Subsequently, 4NADA was copolymerized into a Kapton-type polyimide. We found that low-level introduction of 4NADA (4%) afforded a spectrally BPI film that maintained the electrical insulation and heat resistance properties of polyimide. This method, equivalent to embedding a black monomer in polyimide chains, has merits of economy, universality, process consistency, ready accessibility, and superior performance.

更新日期：2021-10-26

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