乙酯官能化聚酰亚胺的热致重排及其对CO<sub>2</sub>的吸附性能

doi:10.11901/1005.3093.2018.280

材料研究学报

2019, Vol. 33

Issue (3): 209-217 DOI: 10.11901/1005.3093.2018.280

本期目录 | 过刊浏览

乙酯官能化聚酰亚胺的热致重排及其对CO₂的吸附性能

鲁云华¹(

),肖国勇¹,李琳²,董岩¹,迟海军¹,胡知之¹,王同华²(

)

1. 辽宁科技大学化学工程学院鞍山 114051
2. 大连理工大学化工学院精细化工国家重点实验室大连 116024

Thermal Rearrangement of Acetate-functionalized Polyimides and Adsorption Properties for CO₂

Yunhua LU¹(

),Guoyong XIAO¹,Lin LI²,Yan DONG¹,Haijun CHI¹,Zhizhi HU¹,Tonghua WANG²(

)

1. School of Chemical Engineering, University of Science and Technology Liaoning, Anshan 114051, China
2. State Key Lab of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China

引用本文:

鲁云华,肖国勇,李琳,董岩,迟海军,胡知之,王同华. 乙酯官能化聚酰亚胺的热致重排及其对CO₂的吸附性能[J]. 材料研究学报, 2019, 33(3): 209-217.
Yunhua LU, Guoyong XIAO, Lin LI, Yan DONG, Haijun CHI, Zhizhi HU, Tonghua WANG. Thermal Rearrangement of Acetate-functionalized Polyimides and Adsorption Properties for CO₂[J]. Chinese Journal of Materials Research, 2019, 33(3): 209-217.

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摘要:

先使两种含有邻羟基和大体积结构的二胺单体3,3’-二氨基-4,4’-二羟基四苯基甲烷(DDTPM)和9,9-双(3-氨基-4-羟基苯基)芴(BAHPF)分别与六氟二酐(6FDA)进行低温溶液缩聚反应并经化学酰亚胺化得到两种乙酯官能化的聚酰亚胺(PI)，然后在425℃氮气氛围中进行热处理制备出相应的热致重排(TR)聚合物。使用红外光谱仪(FTIR)、核磁共振波谱仪(NMR)、热重分析仪(TGA)、差示扫描量热仪(DSC)、X-射线光电子能谱(XPS)、X-射线衍射仪(XRD)以及Autosorb iQ2等手段表征两种PI和TR聚合物的结构和性能，研究了乙酯官能化聚酰亚胺的热致重排及其CO₂吸附性能。结果表明：PI(DDTPM-6FDA)和PI(BAHPF-6FDA)都发生了部分热致重排反应，且含有两个苯基的PI比含有芴基的PI具有更宽的重排温度范围。它们均具有较高的玻璃化转变温度(T_g)和较宽的晶面间距。TR(DDTPM-6FDA)和TR(BAHPF-6FDA)的比表面积分别为198和582 m²/g，孔径为0.42和0.44 nm，均为微孔聚合物材料，后者对CO₂的吸附能力更强。

关键词 ：有机高分子材料, 聚酰亚胺, 热致重排聚合物, 乙酯官能化, CO₂吸附

Abstract：

Two kinds of diamines containing ortho-hydroxyl groups and bulky moiety, 3,3'-diamino-4,4'-dihydroxytetraphenylmethane (DDTPM) and 9,9-bis (3-amino-4-hydroxyphenyl) fluorene (BAHPF) were polymerized respectively with aromatic dianhydride 2,2-bis (3,4-dicarboxyphenyl) hexafluoropropane dianhydride (6FDA) via a low-temperature solution polymerization, and next, two acetate-functionalized polyimides (PI) were prepared via chemical imidization, and thirdly, which were further thermally treated at 425^oC in N₂ atmosphere to obtain the thermally rearranged polymers. Then, the structure and property of the PIs and TR polymers were characterized by means of Fourier transform infrared spectroscopy (FTIR), nuclear magnetic resonance (NMR), thermogravimetric analysis (TGA), differential scanning calorimeter (DSC), X-ray photoelectric spectroscopy (XPS), X-ray diffraction(XRD) and gas adsorption isotherms etc. The results show that the thermal rearrangement (TR) occured partially for both of the PI(DDTPM-6FDA) and PI(BAHPF-6FDA), and the PI containing two phenyl groups show a range of thermal rearrangement temperature broader than the PI containing fluorene moieties. They show high glass transitionn temperatures (T_g) and larger interplanar crystal spacing. After the thermal treatment at 425^oC, the specific surface area of TR(DDTPM-6FDA) and TR(BAHPF-6FDA) are 198 and 582 m²/g, and their pore diameters are 0.42 and 0.44 nm, respectively. They are belong to microporous materials, and the adsorption capacity for CO₂ of TR(BAHPF-6FDA) is higher than that of TR(DDTPM-6FDA).

Key words： organic polymer materials polyimides thermally rearranged polymers acetate-func-tional CO₂ adsorption

收稿日期: 2018-04-18

ZTFLH:

TB 324

基金资助:国家自然科学基金(21878033);国家自然科学基金(21506020);国家自然科学基金(21406102);国家自然科学基金(21676044);辽宁省自然科学基金(20180550439);辽宁省教育厅优秀人才项目(LJQ2015053)

作者简介: 鲁云华，女，1977年生，副教授

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https://www.cjmr.org/CN/10.11901/1005.3093.2018.280 或 https://www.cjmr.org/CN/Y2019/V33/I3/209

图1 3,3’-二氨基-4,4’-二羟基四苯基甲烷的合成路线

图2 热致重排聚合物的制备过程

图3 二羟基化合物、二硝基化合物和二胺的红外光谱

图4 二羟基化合物、二硝基化合物和二胺的核磁谱

图5 乙酯官能化聚酰亚胺及其热致重排聚合物的红外光谱

图6 乙酯官能化的聚酰亚胺的热重分析曲线

图7 两种乙酯官能化的聚酰亚胺的DSC曲线

图8 热致重排聚合物的XPS分析

图9 乙酯官能化聚酰亚胺及其热致重排聚合物的XRD曲线

图10 热致重排聚合物的SEM照片

表1 乙酯官能化的聚酰亚胺及其热致重排聚合物的溶解性

图11 热致重排聚合物的N2吸附-脱附等温线

图12 热致重排聚合物的CO2吸附等温线

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