新型聚(酰胺-脲-酰亚胺)反渗透复合膜的稳定性

doi:10.7503/cjcu20141084

高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (4): 765.doi: 10.7503/cjcu20141084

新型聚(酰胺-脲-酰亚胺)反渗透复合膜的稳定性

吴丽项¹, 蔡志彬¹, 陈晓林¹, 刘立芬²(), 朱丽芳³(), 高从堦²

1. 浙江工业大学化学工程学院
2. 海洋学院, 杭州 310014
3. 浙江水利水电学院, 杭州 310018

收稿日期:2014-12-08 出版日期:2015-04-10 发布日期:2015-03-19
作者简介:联系人简介: 刘立芬, 女, 博士, 副研究员, 主要从事膜分离技术研究. E-mail: lifenliu@zjut.edu.cn. 朱丽芳, 女, 副教授, 主要从事膜分离技术研究. E-mail: 523274382@qq.com
基金资助:
国家自然科学基金(批准号: 21006096)、浙江省自然科学基金(批准号: LY13B060006)和国家重点基础研究发展计划项目(批准号: 2009CB623402CB615700)资助

Stability of a Novel Poly(amide-urea-imide) Composite Reverse Osmosis Membrane^†

WU Lixiang¹, CAI Zhibin¹, CHEN Xiaolin¹, LIU Lifen^2,^*(), ZHU Lifang^3,^*(), GAO Congjie²

1. College of Chemical Engineering
2. Ocean College, Zhejiang University of Technology, Hangzhou 310014, China
3. Zhejiang University of Water Resources and Electric Power, Hangzhou 310018, China

Received:2014-12-08 Online:2015-04-10 Published:2015-03-19
Contact: LIU Lifen,ZHU Lifang E-mail:lifenliu@zjut.edu.cn;523274382@qq.com
Supported by:
† Supported the National Natural Science Foundation of China(No.21006096), the Zhejiang Provincial Natural Science Foundation of China(No.LY13B060006) and the National Basic Research Program of China(No.2009CB623402CB615700)

摘要/Abstract

摘要：

通过二次界面聚合法制备了一种新型的聚(酰胺-脲-酰亚胺)反渗透复合膜. 将常规二元胺——间苯二胺(MPD)与关键功能单体5-异氰酸酯基-异肽酰氯(ICIC)通过界面聚合得到MPD-ICIC初生态基膜, 再与关键功能单体N,N'-二甲基间苯二胺(DMMPD)经二次界面聚合制得聚(酰胺-脲-酰亚胺)反渗透复合膜. 采用傅里叶变换红外光谱和X射线光电子能谱分析膜活性层的化学结构, 评价膜的分离性能, 在此基础上采用分子动力学模拟方法从微观角度分析二次聚合膜的稳定性.

关键词: 分子动力学, 聚(酰胺-脲-酰亚胺), 反渗透复合膜, 稳定性, N,N'-二甲基间苯二胺, 二次界面聚合

Abstract:

A novel poly(amide-urea-imide) composite reverse osmosis membrane was fabricated via two-step interfacial polymerization. First, 5-isocyanato-isophthaloyl chloride(ICIC) as a key functional monomer reacted with m-phenylenediamine(MPD) to prepare the initial substrate MPD-ICIC membrane by single interfacial polymerization technology. Then, the other key functional monomer N,N'-dimethyl-m-phenylenediamine(DMMPD) was polymerized with the remaining ICIC and acyl chlorine group(—COCl) or isocyanato group(—N=C=O) of the substrate membrane to obtain the new poly(amide-urea-imide) composite reverse osmosis membrane(MPD-ICIC@ICIC-DMMPD) after heat-curing and water rinse. The surface chemical structure of membrane active layer was analyzed by combination of attenuated total reflectance infrared and X-ray photoelectronic spectroscopy, and the separation performance of membrane was also measured. Then, the stability of the obtained membrane MPD-ICIC@ICIC-DMMPD was further analyzed microscopically by molecular dynamic simulation method.

Key words: Molecular dynamic simulation, Poly(amide-urea-imide), Reverse osmosis membrane, Membrane stability, N,N'-Dimethyl-m-phenylenediamine, Two-step interfacial polymerization

中图分类号:

O631
TQ028.8

TrendMD:

吴丽项, 蔡志彬, 陈晓林, 刘立芬, 朱丽芳, 高从堦. 新型聚(酰胺-脲-酰亚胺)反渗透复合膜的稳定性. 高等学校化学学报, 2015, 36(4): 765.

WU Lixiang, CAI Zhibin, CHEN Xiaolin, LIU Lifen, ZHU Lifang, GAO Congjie. Stability of a Novel Poly(amide-urea-imide) Composite Reverse Osmosis Membrane^†. Chem. J. Chinese Universities, 2015, 36(4): 765.

图/表 7

Fig.1 Structures of used monomers

Fig.2 IR spectra of ICIC(A), MPD(a), DMMPD(b)(B) and ATR-FTIR spectrum of MPD-ICIC-DMMPD membrane(C)

Table 1 Elemental composition of the possible ideal structures of polymer chains of the active layer and the actual data of XPS analysis of the MPD-ICIC@ICIC-DMMPD membranes

Calculated data from ideal atructure		Elemental anal.(%)			C/N	C/O	C/N
Calculated data from ideal atructure		C			C/N	O	N
MPD-ICIC	Totally cross-linked(A)	72.0	12.0	16.0	4.50	6.00	0.75
	Linear with pendant—NH₂(B)	73.7	10.5	15.8	4.66	7.02	0.66
	Linear with pendant—COOH(C)	68.2	18.2	13.6	5.01	3.75	1.34
	Linear with pendant—NH₂ and —COOH(D)	70.7	14.6	14.6	4.84	4.84	1.00
ICI-DMMPD	Totally cross-lined(E)	75.0	10.7	14.3	5.25	7.00	0.75
	Linear with pendant—NH₂(F)	76.2	9.5	14.3	5.33	8.00	0.67
	Linear with pendant—COOH(G)	70.8	16.7	12.5	5.67	4.25	1.33
	Linear with pendant—NH₂ and —COOH(H)	73.3	13.3	13.4	5.50	5.50	1.00
MPD-ICI@ICIC-DMMPD membrane(XPS analysis)		72.9	11.5	15.6	4.67	6.34	0.73

Fig.3 Repeating structure cell of MPD-ICIC and ICIC-DMMPD macromolecule chains of the MPD-ICIC@ICIC-DMMPD membrane(X: —NHCONH; Y: —NH2; Z: —COOH)

Fig.4 Separation performance of the MPD-ICIC@ICIC-DMMPD membrane

Fig.5 Interactional energy system of MPD-ICIC@ICIC-DMMPD in the equilibrium state

Fig.6 Interactional energy of MPD-ICIC@ICIC-DMMPD system L-J-D denotes the van der Waals force, and Coul-G represents the electrostatic force.

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新型聚(酰胺-脲-酰亚胺)反渗透复合膜的稳定性

Stability of a Novel Poly(amide-urea-imide) Composite Reverse Osmosis Membrane^†

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新型聚(酰胺-脲-酰亚胺)反渗透复合膜的稳定性

Stability of a Novel Poly(amide-urea-imide) Composite Reverse Osmosis Membrane†

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Stability of a Novel Poly(amide-urea-imide) Composite Reverse Osmosis Membrane^†