薄层复合膜的纳米改性：设计、制备及应用

doi:10.16085/j.issn.1000-6613.2018-1134

化工进展 ›› 2019, Vol. 38 ›› Issue (01): 365-381.DOI: 10.16085/j.issn.1000-6613.2018-1134

薄层复合膜的纳米改性：设计、制备及应用

李猛^1,²(),姚宇健^1,²,张轩^1,²(),王连军^1,²()

1. 南京理工大学环境与生物工程学院，江苏省化工污染控制与资源化重点实验室，江苏南京 210094
2. 南京理工大学环境与生物工程学院，新型膜材料工业和信息化部重点实验室，江苏南京 210094

收稿日期:2018-05-31 修回日期:2018-10-09 出版日期:2019-01-05 发布日期:2019-01-05
通讯作者: 张轩,王连军
作者简介:李猛（1990—），男，博士研究生，从事分离膜的研究。E-mail: <email>Lemon_go8@163.com</email>。|张轩，副教授，博士生导师，研究方向为高分子复合膜的分子设计及应用。E-mail:<email>xuanzhang@njust.edu.cn</email>|王连军，教授，博士生导师，研究方向为膜分离技术在水处理方面的应用。E-mail:<email>wanglj@njust.edu.cn</email>
基金资助:
国家自然科学基金面上项目(21774058，51778292);江苏省优秀青年基金项目(BK20180072);省部共建分离膜与膜过程国家重点实验室（天津工业大学）开放课题(M2-201604);江苏省研究生科研与实践创新计划(KYCX18_0480);国家自然科学基金面上项目（21774058，51778292）；江苏省优秀青年基金项目（BK20180072）；省部共建分离膜与膜过程国家重点实验室（天津工业大学）开放课题（M2-201604）；江苏省研究生科研与实践创新计划（KYCX18_0480）。

Nanomaterials for enhancing thin-film composite: design, fabrication, and application

Meng LI^1,²(),Yujian YAO^1,²,Xuan ZHANG^1,²(),Lianjun WANG^1,²()

1. Key Laboratory of Jiangsu Province for Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science & Technology, Nanjing 210094, Jiangsu, China
2. Key Laboratory of New Membrane Materials, Ministry of Industry and Information Technology, School of Environmental and Biological Engineering, Nanjing University of Science & Technology, Nanjing 210094, Jiangsu, China

Received:2018-05-31 Revised:2018-10-09 Online:2019-01-05 Published:2019-01-05
Contact: Xuan ZHANG,Lianjun WANG

摘要/Abstract

摘要：

以纳滤、反渗透、正渗透为代表的膜技术是目前高端水回用和海水淡化领域的主要技术，但是能源消耗高、分离效率低以及防污抗菌性差等已成为制约膜技术全面应用的主要因素。本文以薄层复合膜为讨论对象，以纳米材料对膜结构和性能的影响为主线，详细介绍了不同类型纳米材料的种类及选取原则、纳米材料的掺杂方式以及掺杂过程中可能遇到的主要问题及解决方法。指出薄层复合膜的纳米改性不仅可以优化膜结构及其物理化学性质（如亲水性、孔隙率、电荷密度、热和机械稳定性），还可以赋予膜某些特定的功能（如抗菌、光催化或吸附能力），从而满足特定的水处理应用需求。最后指出克服纳米材料团聚、解决分散性及相容性的问题是开发新一代高性能分离膜未来的主要研究方向。

关键词: 分离膜, 纳米改性, 渗透率, 选择性, 稳定性, 浓差极化

Abstract:

Membrane-based filtration is the current leading technology for high-end water treatment processes. Nevertheless, the high energy consumption, the “trade-off”relationship between permeability and selectivity, and the low antifouling/antibacterial properties of membranes are challenges that hinder their widespread industrial-scale application. This review summarizes state-of-the-art nanomaterials and the selection principles of them for the fabrication of nanocomposite membranes. An overview on the desalination properties, including separation performance, antifouling/antibacterial characteristics, chlorine resistance, concentration polarization effect, are compared and summarized. Challenges, future research directions, and perspectives on developing high performance nanocomposite membranes are illustrated in detail. It is implicated that more efforts are still needed for the development of next-generation desalination membranes, particularly in the agglomeration, dispersibility, and compatibility of the nanomaterials.

Key words: separation membrane, nano-modification, permeability, selectivity, stability, concentration polarization

中图分类号:

TQ028.8

李猛, 姚宇健, 张轩, 王连军. 薄层复合膜的纳米改性：设计、制备及应用[J]. 化工进展, 2019, 38(01): 365-381.

Meng LI, Yujian YAO, Xuan ZHANG, Lianjun WANG. Nanomaterials for enhancing thin-film composite: design, fabrication, and application[J]. Chemical Industry and Engineering Progress, 2019, 38(01): 365-381.

图/表 7

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纳米材料	掺杂层	制备方法	性能表现	文献
Ag NPs	PA活性层	界面聚合	通量及盐截留变化不大，抗菌性提高	[90]
Ag NPs	PA活性层	界面聚合	膜表面亲水性增强，膜通量及抗菌性提高，盐截留率基本不变	[45]
SMW CNTs	PA活性层	界面聚合	TFN-0.01%膜的纯水渗透系数高达13.2L/(m²·h·bar)，是原始TFC膜的1.6倍，并且对硫酸钠的截留率达到96.8%；此外，以BSA作为特征污染物，改性膜的FRR达到91.2%。高于TFC膜（82%），具有良好的抗污染性能	[62]
ZIF-8/GO	PA活性层	界面聚合	通量提高52%，盐截留几乎不变。具有较好的抗菌性，对大肠杆菌灭菌性达到84.4%	[95]
HNTs	PA活性层	界面聚合	抗污性提高。以BSA作为特征污染物，改性膜的FRR>96%	[106]
GODs	PA活性层	界面聚合	膜表面亲水性增强，改性膜通量是普通膜的6.8倍。以BSA作为特征污染物，改性膜的水通量下降率（DRt）为24.7%， FRR为91.9%，抗污性明显增强	[107]
TiO₂@GO	PA活性层	界面聚合	亲水性增强；在BSA污染下，最优改性膜DRt为24%， FRR>95%	[108]
GO-ODA	PA活性层	界面聚合	纯水渗透系数8.3L/(m²·h·bar)。耐氯性： 3000μL/L NaClO, pH=8, 3h, 改性后的TFC对硫酸钠的截留仍保持在90%以上	[109]
GO	PA活性层	界面聚合	膜表面粗糙度下降，亲水性及水通量提升。耐氯性： 2000μL/L, pH=7, 24h, 改性后的膜对氯化钠截留基本不变， 99.2%	[110]
rGO/TiO₂	PA活性层	界面聚合	亲水性、荷负电性增强；抗污性增强，DRt仅为25%。耐氯性： 2000mg/L NaClO, pH=4, 改性后的RO膜对氯化钠的截留率仅降低3%，而原始膜则降低了30%	[111]
GO	PA活性层表面	表面沉积	抗菌性明显增强，对大肠杆菌的灭菌率达到64.5%	[94]
GO	PA活性层表面	表面沉积	耐氯性： 6000μL/L， pH=11, 2h后氯化钠截留从95.3%降到91.6%； 16h后氯化钠截留降到75%	[112]
GO	PA活性层表面	层层组装	膜表面亲水性增强，粗糙度降低，抗污耐氯性能增强	[70]
GO/Ag	PA活性层表面	化学接枝	膜表面亲水性增强，水接触角小于25°；对大肠杆菌的灭活率超过95%	[113]
SCNTs	PA活性层表面	化学接枝	抗菌性能明显增强，对大肠杆菌灭菌率超过60%	[114]
Ag NPs	PA活性层表面	化学接枝	通量、盐截留几乎不变，抗菌性明显增强	[15]
GO	PSF支撑层	相转化	GO最佳掺量0.25%（质量分数）时， PSF支撑层S值降低，仅为191μm	[115]
CN/rGO	PES支撑层	相转化	CN/rGO最佳掺量0.5%（质量分数）时， PES支撑层S值降低到163μm， J _w比未改性膜提升20%	[116]
TiO₂	PSF支撑层	相转化	改性后PSF支撑层亲水性、孔隙率增加。掺量为1%时， S值最小，为260μm，正渗透性能提升。但高掺量的情况下(0.75%，1%)膜的J _s上升严重	[103]
MOFs	PAN支撑层	相转化	多种MOF材料添加到PAN支撑层中均增大了支撑层的孔隙率，其中PMSC300最为明显，其S值降为190μm左右	[117]
HTNs	PSF支撑层	相转化	支撑层孔隙率、亲水性明显增加， S值为370μm	[118]

纳米材料	掺杂层	制备方法	性能表现	文献
Ag NPs	PA活性层	界面聚合	通量及盐截留变化不大，抗菌性提高	[90]
Ag NPs	PA活性层	界面聚合	膜表面亲水性增强，膜通量及抗菌性提高，盐截留率基本不变	[45]
SMW CNTs	PA活性层	界面聚合	TFN-0.01%膜的纯水渗透系数高达13.2L/(m²·h·bar)，是原始TFC膜的1.6倍，并且对硫酸钠的截留率达到96.8%；此外，以BSA作为特征污染物，改性膜的FRR达到91.2%。高于TFC膜（82%），具有良好的抗污染性能	[62]
ZIF-8/GO	PA活性层	界面聚合	通量提高52%，盐截留几乎不变。具有较好的抗菌性，对大肠杆菌灭菌性达到84.4%	[95]
HNTs	PA活性层	界面聚合	抗污性提高。以BSA作为特征污染物，改性膜的FRR>96%	[106]
GODs	PA活性层	界面聚合	膜表面亲水性增强，改性膜通量是普通膜的6.8倍。以BSA作为特征污染物，改性膜的水通量下降率（DRt）为24.7%， FRR为91.9%，抗污性明显增强	[107]
TiO₂@GO	PA活性层	界面聚合	亲水性增强；在BSA污染下，最优改性膜DRt为24%， FRR>95%	[108]
GO-ODA	PA活性层	界面聚合	纯水渗透系数8.3L/(m²·h·bar)。耐氯性： 3000μL/L NaClO, pH=8, 3h, 改性后的TFC对硫酸钠的截留仍保持在90%以上	[109]
GO	PA活性层	界面聚合	膜表面粗糙度下降，亲水性及水通量提升。耐氯性： 2000μL/L, pH=7, 24h, 改性后的膜对氯化钠截留基本不变， 99.2%	[110]
rGO/TiO₂	PA活性层	界面聚合	亲水性、荷负电性增强；抗污性增强，DRt仅为25%。耐氯性： 2000mg/L NaClO, pH=4, 改性后的RO膜对氯化钠的截留率仅降低3%，而原始膜则降低了30%	[111]
GO	PA活性层表面	表面沉积	抗菌性明显增强，对大肠杆菌的灭菌率达到64.5%	[94]
GO	PA活性层表面	表面沉积	耐氯性： 6000μL/L， pH=11, 2h后氯化钠截留从95.3%降到91.6%； 16h后氯化钠截留降到75%	[112]
GO	PA活性层表面	层层组装	膜表面亲水性增强，粗糙度降低，抗污耐氯性能增强	[70]
GO/Ag	PA活性层表面	化学接枝	膜表面亲水性增强，水接触角小于25°；对大肠杆菌的灭活率超过95%	[113]
SCNTs	PA活性层表面	化学接枝	抗菌性能明显增强，对大肠杆菌灭菌率超过60%	[114]
Ag NPs	PA活性层表面	化学接枝	通量、盐截留几乎不变，抗菌性明显增强	[15]
GO	PSF支撑层	相转化	GO最佳掺量0.25%（质量分数）时， PSF支撑层S值降低，仅为191μm	[115]
CN/rGO	PES支撑层	相转化	CN/rGO最佳掺量0.5%（质量分数）时， PES支撑层S值降低到163μm， J _w比未改性膜提升20%	[116]
TiO₂	PSF支撑层	相转化	改性后PSF支撑层亲水性、孔隙率增加。掺量为1%时， S值最小，为260μm，正渗透性能提升。但高掺量的情况下(0.75%，1%)膜的J _s上升严重	[103]
MOFs	PAN支撑层	相转化	多种MOF材料添加到PAN支撑层中均增大了支撑层的孔隙率，其中PMSC300最为明显，其S值降为190μm左右	[117]
HTNs	PSF支撑层	相转化	支撑层孔隙率、亲水性明显增加， S值为370μm	[118]

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薄层复合膜的纳米改性：设计、制备及应用

Nanomaterials for enhancing thin-film composite: design, fabrication, and application

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