Simultaneously enhanced CO2 permeability and CO2/N2 selectivity at sub-ambient temperature from two novel functionalized intrinsic microporous polymers

选择性 渗透 微型多孔材料 溶解度 聚合物 巴勒 磁导率 化学 化学工程 高分子化学 有机化学 催化作用 生物化学 工程类
作者
Yatao Weng,Wenhui Ji,Chao Ye,Hao Dong,Zhe Gao,Jianxin Li,Chen Luo,Xiaohua Ma
出处
期刊:Journal of Membrane Science [Elsevier BV]
卷期号:644: 120086-120086 被引量:19
标识
DOI:10.1016/j.memsci.2021.120086
摘要

Most polymeric membranes are suffering from CO 2 permeability and CO 2 /N 2 selectivity trade-off effect. Here, a novel anti-trade-off effect by simultaneously increase CO 2 permeability and CO 2 /N 2 selectivity upon decreasing temperature was observed for two new functionalized fully carbon main chain PIMs (HSBI-4-CF 3 and HSBI-3-CF 3 ). They are synthesized by one-step Friedel-Crafts polycondensation reaction from cheap raw materials of 3,3,3’,3’-tetramethyl spirobisindane-6,6’-diol and 3(4)-trifluoromethylbenzaldehyde isomers. Both PIMs showed high molecular weight, good solubility, thermal and mechanical properties. HSBI-4-CF 3 exhibited a higher BET surface area (318 vs 287 m 2 g -1 ) and more open chain packing than HSBI-3-CF 3 . The two polymers showed modest permeability and selectivity as well as pressure and aging resistance. The HSBI-4-CF 3 showed higher permeability but less gas pair selectivity than HSBI-3-CF 3 . Interestingly, upon decreasing temperature to −20 °C, both polymers showed improved CO 2 permeability and CO 2 /N 2 selectivity at the same time. The CO 2 permeability of HSBI-3-CF 3 increased from 292 to 453 Barrer and the CO 2 /N 2 selectivity improved from 20.3 to 44.0. The higher permeability at low temperature was attributed to the increased solubility (S CO2 ∼ 3.2 fold) over diffusion coefficient drop (D CO2 ∼ 2.1 times) of CO 2 , which is opposite to that of N 2 , and thus enhanced the CO 2 /N 2 selectivity. The origin of this effect comes from their minus activation energy of permeation (E p ) of CO 2 (−0.78 and −1.1 kcal mol -1 ) while positive E p for N 2 (1.7 and 1.1 kcal mol -1 ), which is due to the diffusion activation energy (E d ) overweight the heat of sorption (-H s ) for N 2 while inverse for CO 2 . This unique simultaneously increase CO 2 permeability and CO 2 /N 2 selectivity opened a new era in membrane-based sub-ambient temperature CO 2 capture. • Two novel –OH and –CF 3 functionalized PIMs with fully carbon backbone were synthesized from two isomer monomers. • The polymerization is a one-step reaction from cheap materials and easy scale-up. • The two polymers showed simultaneously improved P CO2 and a CO2/N2 upon decreasing temperature. • The increased P CO2 is originated from the enhanced S CO2 at low temperature. • The increased P CO2 and decreased P N2 at low temperature caused the improved a CO2/N2 .
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