氯化聚氯乙烯复合纳滤膜的制备及其在模拟RB5染料废水处理中的应用

doi:10.16085/j.issn.1000-6613.2021-0088

摘要/Abstract

摘要：

以氯化聚氯乙烯（CPVC）超滤膜为基膜，采用单宁酸（TA）和哌嗪（PIP）在CPVC膜表面共沉积后与交联剂均苯三甲酰氯（TMC）进行界面聚合得到PA/TA/CPVC复合纳滤膜，采用扫描电镜（SEM）、原子力显微镜（AFM）、红外光谱及接触角对PA/TA/CPVC复合纳滤膜进行了表征，并探讨了干燥时间、TA/PIP浓度比、TA+PIP总浓度、TMC浓度对PA/TA/CPVC复合纳滤膜微观结构与性能的影响。结果表明，TA/PIP浓度比最佳为7/3，TA/PIP层的最佳干燥时间为20min，PA/TA/CPVC复合纳滤膜的纯水通量随着TA+PIP总浓度的增加和TMC浓度的增加而减少，对PEG1000的截留率均在90%以上。PA/TA/CPVC复合纳滤膜纯水通量最大值为4.5L/(m² · h · bar)，此时PEG1000的截留率达到95.8%。对模拟RB5染料废水的最大通量为4.3L/(m² · h · bar)，此时RB5的截留率为95.4%，对模拟RB5染料废水的稳定性较好。

关键词: 氯化聚氯乙烯复合纳滤膜, 单宁酸/哌嗪, 共沉积和界面聚合组合法, 模拟RB5染料废水

Abstract:

Using CPVC (chlorinated polyvinyl chloride) ultrafiltration membrane as the base membrane, after co-deposition of TA (tannic acid) and PIP (piperazine) on the surface of the CPVC membrane, interfacial polymerization is carried out with the crosslinking agent TMC (trimesoyl chloride) to obtain a PA/TA/CPVC composite nanofiltration membrane, the PA/TA/CPVC composite nanofiltration membrane was characterized by SEM, AFM, FTIR and contact angle, the effects of drying time, TA/PIP concentration ratio, TA+PIP total concentration, and TMC concentration on the microstructure and performance of PA/TA/CPVC composite nanofiltration membranes were discussed. The research results show that the best TA/PIP concentration ratio is 7/3, the best drying time of the TA/PIP layer is 20min, and the pure water flux of the PA/TA/CPVC composite nanofiltration membrane increases with the increase of TA+PIP total concentration and the concentration of TMC The rejection rate of PEG1000 is above 90%. The maximum pure water flux of PA/TA/CPVC composite nanofiltration membrane is 4.5 L/(m² · h · bar), and the rejection rate of PEG1000 reaches 95.8%. The maximum flux to the simulated RB5 dye wastewater is 4.3 L/(m² · h · bar), and the rejection rate of RB5 at this time is 95.4%, which shows good stability to the simulated RB5 dye wastewater.

Key words: CPVC composite nanofiltration membrane, TA/PIP, co-deposition and interfacial polymerization combined method, simulated RB5 dye wastewater

中图分类号:

X703

李泽辉, 崔恒, 王军. 氯化聚氯乙烯复合纳滤膜的制备及其在模拟RB5染料废水处理中的应用[J]. 化工进展, 2021, 40(S1): 456-465.

LI Zehui, CUI Heng, WANG Jun. Preparation of CPVC composite nanofiltration membrane and its application in simulated RB5 dye wastewater treatment[J]. Chemical Industry and Engineering Progress, 2021, 40(S1): 456-465.

图/表 11

图1 PA/TA/CPVC复合纳滤膜、CPVC以及TA和PIP的FTIR光谱图

图2 制备条件对PA/TA/CPVC复合纳滤膜微观结构和表面粗糙度的影响

图3 干燥时间对PA/TA/CPVC复合纳滤膜的过滤性能的影响及纯水通量衰减情况

图4 TA/PIP浓度比对PA/TA/CPVC复合纳滤膜表面水接触角的影响、过滤性能的影响及纯水通量衰减情况

图5 TA+PIP总浓度对PA/TA/CPVC复合纳滤膜过滤性能的影响及纯水通量衰减情况

图6 TMC浓度对PA/TA/CPVC复合纳滤膜的过滤性能的影响及纯水通量衰减情况

图7 干燥时间对PA/TA/CPVC复合纳滤膜处理模拟RB5染料废水过滤效果的影响

图8 TA/PIP浓度比对PA/TA/CPVC复合纳滤膜处理模拟RB5染料废水过滤效果的影响

图9 TA+PIP总浓度对PA/TA/CPVC复合纳滤膜处理模拟RB5染料废水过滤效果的影响

图10 TMC浓度对PA/TA/CPVC复合纳滤膜处理模拟RB5染料废水过滤效果的影响

图11 PA/TA/CPVC复合纳滤膜处理模拟RB5染料废水的稳定性探讨（3种膜干燥时间均为20min，TA/PIP浓度比均为7/3，其中a：TA+PIP总浓度为0.5g/L，TMC浓度为1g/L；b：TA+PIP总浓度为0.6g/L，TMC浓度为1g/L；c：TA+PIP总浓度为0.5g/L， TMC浓度为0.7g/L）

参考文献 36

1	FAN L, MA Y, SU Y, et al. Green coating by coordination of tannic acid and iron ions for antioxidant nanofiltration membranes [J]. RSC Advances, 2015, 5(130): 107777-107784.
2	LI Q, LIAO Z, FANG X, et al. Tannic acid-polyethyleneimine crosslinked loose nanofiltration membrane for dye/salt mixture separation [J]. Journal of Membrane Science, 2019, 584: 324-332.
3	HE M, SUN H, SUN H, et al. Non-organic solvent prepared nanofiltration composite membrane from natural product tannic acid (TA) and cyclohexane-1,4-diamine (CHD) [J]. Separation and Purification Technology, 2019, 223: 250-259.
4	WU H, XIE J, MAO L. One-pot assembly tannic acid-titanium dual network coating for low-pressure nanofiltration membranes [J]. Separation and Purification Technology, 2020, 233: 116051-116059.
5	ZHANG H, GONG X Y, LI W X, et al. Thin-film nanocomposite membranes containing tannic acid-Fe³⁺ modified MoS₂ nanosheets with enhanced nanofiltration performance [J]. Journal of Membrane Science, 2020, 616: 118605-118612.
6	CHAKRABARTY T, PéREZ-MANRíQUEZ L, NEELAKANDA P, et al. Bioinspired tannic acid-copper complexes as selective coating for nanofiltration membranes [J]. Separation and Purification Technology, 2017, 184: 188-194.
7	XU Y, GUO D, LI T, et al. Manipulating the mussel-inspired co-deposition of tannic acid and amine for fabrication of nanofiltration membranes with an enhanced separation performance [J]. J. Colloid Interface Sci., 2020, 565: 23-34.
8	LU W, SHI D, ZHANG H, et al. Advanced poly(vinyl pyrrolidone) decorated chlorinated polyvinyl chloride membrane with low area resistance for vanadium flow battery [J]. Journal of Membrane Science, 2021, 620: 118947-118962.
9	REN L, CHEN J, LU Q, et al. Construction of high selectivity and antifouling nanofiltration membrane via incorporating macrocyclic molecules into active layer [J]. Journal of Membrane Science, 2020, 597: 117641-117653.
10	ZHANG Z, KANG G, YU H, et al. Fabrication of a highly permeable composite nanofiltration membrane via interfacial polymerization by adding a novel acyl chloride monomer with an anhydride group [J]. Journal of Membrane Science, 2019, 570/571: 403-409.
11	WU D, HUANG Y, YU S, et al. Thin film composite nanofiltration membranes assembled layer-by-layer via interfacial polymerization from polyethylenimine and trimesoyl chloride [J]. Journal of Membrane Science, 2014, 472: 141-153.
12	XU X X, ZHOU C L, ZENG B R, et al. Structure and properties of polyamidoamine/polyacrylonitrile composite nanofiltration membrane prepared by interfacial polymerization [J]. Separation and Purification Technology, 2012, 96: 229-236.
13	CHENG J, SHI W, ZHANG L, et al. A novel polyester composite nanofiltration membrane formed by interfacial polymerization of pentaerythritol (PE) and trimesoyl chloride (TMC) [J]. Applied Surface Science, 2017, 416:152-159.
14	ZENG Y, WANG L, ZHANG L, et al. An acid resistant nanofiltration membrane prepared from a precursor of poly S(-triazine-amine) by interfacial polymerization [J]. Journal of Membrane Science, 2018, 546:225-233.
15	MI Y F, WANG N, QI Q, et al. A loose polyamide nanofiltration membrane prepared by polyether amine interfacial polymerization for dye desalination [J]. Separation and Purification Technology, 2020, 248: 117079-117086.
16	DING J, WU H, WU P. Preparation of highly permeable loose nanofiltration membranes using sulfonated polyethylenimine for effective dye/salt fractionation [J]. Chemical Engineering Journal, 2020, 396: 125199-125209.
17	ZHANG Y, SU Y, PENG J, et al. Composite nanofiltration membranes prepared by interfacial polymerization with natural material tannic acid and trimesoyl chloride [J]. Journal of Membrane Science, 2013, 429: 235-242.
18	WU M, YUAN J, WU H, et al. Ultrathin nanofiltration membrane with polydopamine-covalent organic framework interlayer for enhanced permeability and structural stability [J]. Journal of Membrane Science, 2019, 576: 131-141.
19	LI M, WU L, ZHANG C, et al. Hydrophilic and antifouling modification of PVDF membranes by one-step assembly of tannic acid and polyvinylpyrrolidone [J]. Applied Surface Science, 2019, 483:967-978.
20	XIAO Y, GUO D, LI T, et al. Facile fabrication of superhydrophilic nanofiltration membranes via tannic acid and irons layer-by-layer self-assembly for dye separation [J]. Applied Surface Science, 2020, 515: 146063-146072.
21	LIU H, LIU G, ZHANG M, et al. Rapid preparation of Tannic acid (TA) based zwitterionic nanofiltration membrane via a multiple layer-by-layer (mLBL) assembly strategy for enhanced antifouling performance [J]. Separation and Purification Technology, 2020, 253:117519-117529.
22	CHEN F, DONG S, WANG Z, et al. Preparation of mixed matrix composite membrane for hydrogen purification by incorporating ZIF-8 nanoparticles modified with tannic acid [J]. International Journal of Hydrogen Energy, 2020, 45(12): 7444-7454.
23	XU L, HE Y, FENG X, et al. A comprehensive description of the threshold flux during oil/water emulsion filtration to identify sustainable flux regimes for tannic acid (TA) dip-coated poly(vinylidene fluoride) (PVDF) membranes [J]. Journal of Membrane Science, 2018, 563: 43-53.
24	HU W, CUI X, XIANG L, et al. Tannic acid modified MoS₂ nanosheet membranes with superior water flux and ion/dye rejection [J]. Journal of Colloid and Interface Science, 2020, 560: 177-185.
25	KIM H J, KIM D G, YOON H, et al. Polyphenol/Fe^Ⅲ complex coated membranes having multifunctional properties prepared by a one-step fast assembly [J]. Advanced Materials Interfaces, 2015, 2(14): 1500298-1500305.
26	CHEN S, XIE Y, XIAO T, et al. Tannic acid-inspiration and post-crosslinking of zwitterionic polymer as a universal approach towards antifouling surface [J]. Chemical Engineering Journal, 2018, 337: 122-132.
27	LIM M Y, CHOI Y S, KIM J, et al. Cross-linked graphene oxide membrane having high ion selectivity and antibacterial activity prepared using tannic acid-functionalized graphene oxide and polyethyleneimine [J]. Journal of Membrane Science, 2017, 521: 1-9.
28	LIN C E, ZHOU M Y, HUNG W S, et al. Ultrathin nanofilm with tailored pore size fabricated by metal-phenolic network for precise and rapid molecular separation [J]. Separation and Purification Technology, 2018, 207: 435-442.
29	LI Q, LIAO Z, FANG X, et al. Tannic acid assisted interfacial polymerization based loose thin-film composite NF membrane for dye/salt separation [J]. Desalination, 2020, 479: 114343-114352.
30	LI T, XIAO Y, GUO D, et al. In-situ coating TiO₂ surface by plant-inspired tannic acid for fabrication of thin film nanocomposite nanofiltration membranes toward enhanced separation and antibacterial performance [J]. Journal of Colloid and Interface Science, 2020, 572: 114-121.
31	JIANG C, TIAN L, ZHAI Z, et al. Thin-film composite membranes with aqueous template-induced surface nanostructures for enhanced nanofiltration [J]. Journal of Membrane Science, 2019, 589:117244-117253.
32	ZHANG N, HUANG Z, YANG N, et al. Nanofiltration membrane via EGCG-PEI co-deposition followed by cross-linking on microporous PTFE substrates for desalination [J]. Separation and Purification Technology, 2020, 232: 115964-115973.
33	YANG Y, LI Y, LI Q, et al. Rapid co-deposition of graphene oxide incorporated metal-phenolic network/piperazine followed by crosslinking for high flux nanofiltration membranes [J]. Journal of Membrane Science, 2019, 588: 117203-117212.
34	ZHANG H, BIN L, PAN J, et al. Carboxyl-functionalized graphene oxide polyamide nanofiltration membrane for desalination of dye solutions containing monovalent salt [J]. Journal of Membrane Science, 2017, 539: 128-137.
35	LI Y, SU Y, LI J, et al. Preparation of thin film composite nanofiltration membrane with improved structural stability through the mediation of polydopamine [J]. Journal of Membrane Science, 2015, 476: 10-19.
36	ANG M B M Y, JI Y L, HUANG S H, et al. A facile and versatile strategy for fabricating thin-film nanocomposite membranes with polydopamine-piperazine nanoparticles generated in situ [J]. Journal of Membrane Science, 2019, 579: 79-89.

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