Preparation of polyamide/cellulose acetate thin-film composite forward osmosis membranes and optimization of phase inversion process parameters

doi:10.16085/j.issn.1000-6613.2023-0441

Abstract

Abstract:

Forward osmosis (FO) technology has the advantages of low operating pressure, energy consumption and membrane fouling. It may contribute to solutions to ease the water and energy shortage in the world. However, the lack of stable and high permselective FO membranes has thwarted its wide spread applications. In this paper, starting from adjusting the process parameters of phase inversion, the structure and properties of cellulose acetate (CA) substrates were effectively controlled by changing the kinds of additives and the operation parameters (coating thickness, solvent evaporation time and coagulation bath temperature). Then polyamide (PA) separation layer was formed on the hydrophilic porous CA substrate by interface polymerization (IP) to obtain the thin-film composite FO membrane. The experimental results showed that when the casting solution composed of 10% CA and Porogen A was cast under a 150μm gap and coagulated at 25℃ to form porous CA substrate, the stable TFC-FO membranes could be prepared from IP to have the best permselectivity. With 1mol/L NaCl solution as the drug substance (DS) and deionized water (DIW) as the feed solution (FS), the FO water flux reached 10.94L/(m²·h) under a low reverse salt flux value of 0.0500mol/(m²·h). Its NaCl rejection rate was 95.0% and the structure parameter (S) was 1404μm.

Key words: membranes, forward osmosis, phase inversion, polyamide, cellulose acetate, permeability

摘要：

正渗透（forward osmosis，FO）分离技术具有低操作压力、低能耗、膜污染程度轻等优点，可能成为解决世界上水资源匮乏和能源短缺等极具挑战性问题的潜在方案。然而，正渗透技术缺乏性能优异且稳定的FO膜被认为是限制其发展及应用的主要障碍之一。本文从调控相转化工艺参数出发，通过改变铸膜液中的致孔剂种类以及操作参数（涂布厚度、溶剂蒸发时间和凝固浴温度）来实现对醋酸纤维素（cellulose acetate，CA）基底结构和性能的有效调控，并采用界面聚合（interfacial polymerization，IP）的方法在这种亲水的多孔基底上制备聚酰胺（polyamide，PA）分离层，得到薄膜复合正渗透（TFC-FO）膜。实验结果表明，用10%（质量分数）CA、致孔剂A等组成的铸膜液在150μm浇铸刀下涂布，立即浸入25℃凝固浴相转化制得CA基底，再经界面聚合所得的TFC-FO膜的渗透选择性最佳，以1mol/L NaCl溶液作为汲取液，去离子水作为原料液，膜的FO水通量达10.94L/(m²·h)，反向盐通量为0.0500mol/(m²·h)，对NaCl的截留率为95.0%，结构参数为1404μm。

关键词: 膜, 正渗透, 相转化, 聚酰胺, 醋酸纤维素, 渗透率

CLC Number:

TQ051

LIN Mingjie, LI Shiyang, MA Junmei, GAO Congjie, XUE Lixin. Preparation of polyamide/cellulose acetate thin-film composite forward osmosis membranes and optimization of phase inversion process parameters[J]. Chemical Industry and Engineering Progress, 2024, 43(3): 1418-1427.

林明杰, 李士洋, 马俊梅, 高从堦, 薛立新. 聚酰胺/醋酸纤维素复合正渗透膜的制备及相转化工艺参数的优化[J]. 化工进展, 2024, 43(3): 1418-1427.

Figures/Tables 16

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致孔剂种类	R_NaCl/%	A/L·m^-2·h^-1·bar^-1	B/L·m^-2·h^-1	(B/A)/bar	S/μm
丙酮酸	90.2±0.6	0.76±0.05	0.46±0.07	0.60	2832
致孔剂A	95.0±1.0	4.55±0.47	1.33±0.25	0.29	1404
PEG-800	89.6±2.0	0.93±0.04	0.60±0.11	0.65	2150
PEG-4000	88.3±0.7	0.95±0.01	0.70±0.03	0.74	1429
PEG-20000	85.4±0.5	0.97±0.02	0.92±0.05	0.95	1392

致孔剂种类	R_NaCl/%	A/L·m^-2·h^-1·bar^-1	B/L·m^-2·h^-1	(B/A)/bar	S/μm
丙酮酸	90.2±0.6	0.76±0.05	0.46±0.07	0.60	2832
致孔剂A	95.0±1.0	4.55±0.47	1.33±0.25	0.29	1404
PEG-800	89.6±2.0	0.93±0.04	0.60±0.11	0.65	2150
PEG-4000	88.3±0.7	0.95±0.01	0.70±0.03	0.74	1429
PEG-20000	85.4±0.5	0.97±0.02	0.92±0.05	0.95	1392

涂布厚度	R_NaCl/%	A/L·m^-2·h^-1·bar^-1	B/L·m^-2·h^-1	(B/A)/bar	S/μm
100μm	86.2±0.5	5.80±0.30	5.18±0.39	0.89	1533
150μm	95.0±1.0	4.55±0.47	1.33±0.25	0.29	1404
200μm	96.0±0.2	4.24±0.38	0.98±0.14	0.23	1513
300μm	95.8±0.4	3.75±0.16	0.91±0.07	0.24	1823

涂布厚度	R_NaCl/%	A/L·m^-2·h^-1·bar^-1	B/L·m^-2·h^-1	(B/A)/bar	S/μm
100μm	86.2±0.5	5.80±0.30	5.18±0.39	0.89	1533
150μm	95.0±1.0	4.55±0.47	1.33±0.25	0.29	1404
200μm	96.0±0.2	4.24±0.38	0.98±0.14	0.23	1513
300μm	95.8±0.4	3.75±0.16	0.91±0.07	0.24	1823

蒸发时间	R_NaCl/%	A/L·m^-2·h^-1·bar^-1	B/L·m^-2·h^-1	(B/A)/bar	S/μm
0s	95.0±1.0	4.55±0.47	1.33±0.25	0.29	1404
30s	95.2±0.5	3.20±0.34	0.91±0.20	0.28	1659
60s	96.8±0.5	2.71±0.12	0.51±0.10	0.18	1744
90s	96.9±0.4	2.37±0.08	0.43±0.08	0.18	1994