包含原位生长ZIF-L粒子的PEI基高效染料脱盐混合基质纳滤膜

doi:10.16085/j.issn.1000-6613.2024-0712

化工进展 ›› 2024, Vol. 43 ›› Issue (S1): 431-442.DOI: 10.16085/j.issn.1000-6613.2024-0712

包含原位生长ZIF-L粒子的PEI基高效染料脱盐混合基质纳滤膜

薛立新¹^,²(), 涂龙斗²^,³, 李士洋³, 郑晨晨³, 蔡达健³, 高从堦³

^1.温州大学化学与材料工程学院，浙江温州 325035
^2.温州大学新材料与产业技术研究院，浙江温州 325024
^3.浙江工业大学膜分离与水科学技术研究院，浙江杭州 310014

收稿日期:2024-04-28 修回日期:2024-06-20 出版日期:2024-11-20 发布日期:2024-12-06
通讯作者: 薛立新
作者简介:薛立新（1966—），男，研究员，博士生导师，研究方向为膜科学与技术。E-mail：20230212@wzu.edu.cn。
基金资助:
国家自然科学基金(NSFC-21975222)

High efficient dye desalting mixed matrix nanofiltration membranes containing in-situ grown ZIF-L particles in polyethyleneimine (PEI) coating before interface polymerization

XUE Lixin¹^,²(), TU Longdou²^,³, LI Shiyang³, ZHENG Chenchen³, CAI Dajian³, GAO Congjie³

^1.School of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, Zhejiang, China
^2.Institute of New Materials and Industrial Technology, Wenzhou University, Wenzhou 325024, Zhejiang, China
^3.Center for Membrane Separation and Water Science and Technology, Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China

Received:2024-04-28 Revised:2024-06-20 Online:2024-11-20 Published:2024-12-06
Contact: XUE Lixin

摘要/Abstract

摘要：

沸石咪唑酯骨架（ZIF）因其结构可调、制备简单以及稳定性优异，被认为是突破膜材料上限的最佳材料之一。本文通过在聚乙烯亚胺（PEI）基涂层原位生长ZIF-L粒子，然后与均苯三甲酰氯（TMC）界面聚合，得到了性能良好的染料脱盐混合基质疏松纳滤膜。利用PEI与Zn²⁺的配位作用，保证Zn(Ⅱ)离子的均匀分布，还建立了原位生成ZIF-L纳米粒子与聚酰胺之间的界面连接，避免了界面缺陷的形成。ZIF-L粒子的原位生成增加了膜表面粗糙度，改善了膜表面亲水性能，提供了分离层的水通道，缩短了水运输路径。对于刚果红（CR）/盐混合溶液，与未负载ZIF粒子的PEI/TMC膜相比，PEI(ZIF)/TMC膜在截留率维持不变的情况下，渗透系数提高近17倍，达到68.1~71.7L/(m²·h·bar)，其刚果红染料截留率达到98%，Na₂SO₄和NaCl截留率分别为12.4%和2.7%，截留分离选择系数分别为7.8和36.1。

关键词: 原位生长, 染料/盐分离, ZIF-L, 混合基质纳滤膜, 界面聚合

Abstract:

Zeolitic imidazolate frameworks (ZIFs) are considered to be one of the best materials for breaking through the upper limit of membrane materials due to their structure being adjustable, easy preparation and excellent stability. In this study, a high-performance dye desalination mixed matrix loose nanofiltration membrane was obtained by the in-situ growth of ZIF-L particles on a polyethyleneimine (PEI) based coating and followed by interfacial polymerization with trimesoyl chloride (TMC). Using the coordination action between PEI and Zn²⁺, the uniform distribution of Zn(Ⅱ) ions was ensured and also established an in-situ generation of ZIF-L nanoparticles with the polyamide interface, avoiding the formation of interface defects. The in-situ generation of ZIF-L particles increased the roughness of the membrane surface and improved the surface hydrophilicity, providing a water channel for the separation layer and shortening the water transport path. For the Congo red/salt mixed solution, compared with the PEI/TMC membrane without ZIF particle loading, the PEI(ZIF)/TMC membrane maintained the rejection rate unchanged, while the permeability was increased by nearly 17 times, reaching 68.1—71.7L/(m²·h·bar). The Congo red (CR) rejection rate was 98%. The Na₂SO₄ and NaCl rejection rates were 12.4% and 2.7%, and the separation selectivity coefficients were 7.8 and 36.1, respectively.

Key words: in-situ growth, dye/salt separation, ZIF-L, mixed matrix nanofiltration membrane, interfacial polymerization

中图分类号:

TQ028.8

薛立新, 涂龙斗, 李士洋, 郑晨晨, 蔡达健, 高从堦. 包含原位生长ZIF-L粒子的PEI基高效染料脱盐混合基质纳滤膜[J]. 化工进展, 2024, 43(S1): 431-442.

XUE Lixin, TU Longdou, LI Shiyang, ZHENG Chenchen, CAI Dajian, GAO Congjie. High efficient dye desalting mixed matrix nanofiltration membranes containing in-situ grown ZIF-L particles in polyethyleneimine (PEI) coating before interface polymerization[J]. Chemical Industry and Engineering Progress, 2024, 43(S1): 431-442.

图/表 18

图1 复合膜制备工艺

图2 复合膜傅里叶变换红外光谱图

图3 复合膜XRD表征

图4 复合膜平面及断面SEM图及表面AFM图

图5 PEI(ZIF)/TMC表面元素分布

表1 复合膜EDS元素含量

膜	元素质量分数/%
膜	C	N	O	Zn
PEI(ZIF)	64.0	20.5	12.1	3.4
PEI/TMC	63.9	11.9	24.2	0
PEI(ZIF)/TMC	64.2	13.8	20.5	1.5

图6 ZIF-L负载量对PEI(ZIF)/TMC膜性能的影响

图7 复合膜中ZIF粒子负载量与Zn2+浓度关系

图8 TMC浓度对PEI(ZIF)/TMC膜性能的影响

图9 热处理时间对PEI(ZIF)/TMC膜性能的影响

图10 不同复合膜对CR的分离性能

图11 不同复合膜的水接触角与Zeta电位

图12 PEI(ZIF)/TMC膜单组分染料和盐的分离性能及理想截留选择性

图13 PEI(ZIF)/TMC膜MWCO测试及孔径分布

图14 染料的分子量及截留性能

图15 PEI(ZIF)/TMC膜染料/盐混合溶液分离性能和截留选择性

图16 PEI(ZIF)/TMC膜高浓度盐及不同跨膜压差的分离性能

图17 PEI(ZIF)/TMC膜长期运行稳定性以及抗污染性能

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包含原位生长ZIF-L粒子的PEI基高效染料脱盐混合基质纳滤膜

High efficient dye desalting mixed matrix nanofiltration membranes containing in-situ grown ZIF-L particles in polyethyleneimine (PEI) coating before interface polymerization

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