聚酰亚胺渗透汽化膜用于有机溶剂脱水的改性研究进展

doi:10.16085/j.issn.1000-6613.2023-0846

摘要/Abstract

摘要：

聚酰亚胺有机高分子聚合物结构内含有氢键，且具有良好的耐溶剂性、易成膜性、高力学性能等优点。聚酰亚胺膜有望在渗透汽化有机溶剂脱水领域得到广泛应用。然而，聚酰亚胺膜高分子链间作用力强，链段排列紧密，往往造成溶剂分子渗透困难、渗透通量低等问题，限制其发展。对聚酰亚胺膜开展改性研究，以提高其渗透通量，同时保持高分离因子，是近年来的主要研究方向。本文对渗透汽化膜分离技术进行了概述，介绍了其工作原理及常用分离膜种类。详细综述了近年来用于渗透脱水的聚酰亚胺膜的改性研究进展，重点评述了共混、掺杂、交联和共聚改性，并分析了四种改性方法的作用原理，对分离性能的影响及其优缺点。最后，对聚酰亚胺膜在渗透汽化分离领域未来的发展方向进行展望，指出需揭示聚酰亚胺聚合物链与溶剂分子间的作用机制，解决渗透通量与选择性之间“trade-off”的制约关系。

关键词: 膜分离, 渗透汽化, 聚酰亚胺, 改性, 有机溶剂, 脱水

Abstract:

Polyimide contains hydrogen bonds in organic polymer structure and has good solvent resistance, easy film formation, high mechanical properties, et al. Polyimide membrane is expected to be widely used in the field of pervaporation for organic solvents. However, the strong inter-chain interaction and chain segments packing result in the low flux as the difficult water molecules penetration through the membranes based on them. Therefore, the modification is urgent to improve separation performance of polyimide membranes. In this paper, pervaporation process was summarized systematically including its mechanism and common separation membrane types. The recent research progress in modification methods of polyimide pervaporation membranes was reviewed. Four methods were discussed including blending, doping, cross-linking and copolymerization. The principles of these methods and their influence on separation performance were analyzed. The advantages and disadvantages of the modifications were also summarized. Finally, the development direction of polyimide membrane in the field of pervaporation separation was prospected. It pointed out that the interaction mechanism between polyimide polymer chain and solvent molecule needed to be revealed to solve the "trade-off" restriction between permeation flux and selectivity.

Key words: membrane separation, pervaporation, polyimide, modify, organic solvents, dehydration

中图分类号:

TB383

李妍, 吴芹, 陈康成, 张耀远, 史大昕, 黎汉生. 聚酰亚胺渗透汽化膜用于有机溶剂脱水的改性研究进展[J]. 化工进展, 2024, 43(6): 2915-2927.

LI Yan, WU Qin, CHEN Kangcheng, ZHANG Yaoyuan, SHI Daxin, LI Hansheng. Modified polyimide pervaporation membranes for dehydration of organic solvent[J]. Chemical Industry and Engineering Progress, 2024, 43(6): 2915-2927.

图/表 18

图1 溶解-扩散模型原理图

图2 膜渗透汽化分离过程

图3 真空冷凝渗透汽化过程1—储料罐；2—进料泵；3—转子流量计；4—膜组件；5—渗透汽化管；6—产品收集瓶；7—安全瓶；8—真空泵；9—旁路调节阀；10—温度传感器；11—真空表；12—加热器；13—杜瓦瓶

图4 60℃下cPIM-1负载量对85%异丙醇溶液分离性能的影响[27]

图5 hPIM-1负载量对不同体系分离性能的影响[23]

图6 PBI与PI分子间相互作用示意图[24]

图7 混合基质膜结构示意图和UiO-66-NH2负载量对混合基质膜分离性能的影响[29]

表1 纯PI膜与不同UiO-66-NH2负载量的PI膜的溶剂吸收率[29]

膜材料	UiO-66-NH₂负载量/%	吸水率 /%	甲醇吸收率/%	乙醇吸收率/%	异丙醇吸收率/%
PI	0	3.3±0.3	9.2±0.3	11.5±0.7	18.4±0.6
MMM	10	5.6±0.5	8.0±0.6	8.3±0.3	10.4±0.6
MMM	20	9.4±0.5	6.1±0.9	7.1±0.3	9.8±0.8
MMM	30	16.9±0.7	5.0±0.2	6.5±0.6	8.2±0.8

图8 热诱导PI交联机理[44]

图9 PI膜改性常用的胺交联剂

图10 PDA与PI交联示意图[55]

图11 BTCH与PI交联示意图[56]

图12 醇交联机理图[45]

图13 PI常用共聚单体

图14 聚合物及BHTDA、BATB、BADTB、DBAPB结构示意图[63]

图15 BPADA、MDA、ODA、DAPy、DABA、DBSA结构示意图[64]

图16 P84共聚PI化学结构

图17 PDMS-b-FPI和PDMS-b-PI结构[67]

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