基于二维纳米材料的水处理功能膜研究进展

doi:10.16085/j.issn.1000-6613.2020-1938

摘要/Abstract

摘要：

二维纳米材料是制备膜材料中一类重要的掺杂材料或膜构筑单元，也是新型水处理功能膜的研究热点。已有许多研究报道了二维纳米材料通过有序的堆叠和自组装在膜内构建出规整的水通道，可以赋予膜可调控的分离性能，进而实现trade-off效应的突破，被认为是“下一代膜材料”（next-generation membranes）。同时，二维纳米材料的独特片层结构、催化性能及可修饰性可使膜材料获得新的功能，如导电性能、光/电催化性能等。本文综述了近年来基于二维纳米材料的水处理功能膜研究进展，重点介绍了共混法、自组装等制备方法，并总结了此类功能膜在抗污染、膜通量恢复、强化污染物去除、调控盐截留及污染物监测领域的应用。最后对基于二维纳米材料的水处理功能膜发展方向，如限域催化、调控盐分离、监测传感等新兴领域进行了分析和展望。

关键词: 二维纳米材料, 膜, 功能膜, 催化, 废水, 环境

Abstract:

Two-dimensional nanomaterials are an important category of membrane additives or building blocks, and also a research hotspot of novel functional membranes for water treatment. It has been proved that two-dimensional nanomaterials can construct regular water channels by orderly stacking and self-assembly. The membranes based on two-dimensional nanomaterials are considered as next-generation membranes with tunable separation performance, having the potential of achieving breakthrough of the trade-off effect. Meanwhile, due to the high specific surface area, catalytic ability and modifiability of the two-dimensional nanomaterials, the membranes based on two-dimensional nanomaterials can obtain new functions, such as conductivity, photocatalytic/electrocatalytic properties and so on. In this paper, the research progress of functional membranes based on two-dimensional nanomaterials for water treatment in recent years was reviewed with emphasis on the preparation methods such as blending and self-assembly. The applications of these functional membranes in the fields of antifouling, flux recovery, enhanced pollutant removal, modulating salt rejection and sensing were also summarized. Finally, the development trend of functional membrane based on two-dimensional nanomaterials for water treatment was proposed.

Key words: two-dimensional nanomaterials, membrane, functional membranes, catalysis, waste water, environment

中图分类号:

李胄彦, 戴若彬, 李洋, 王雪野, 王志伟. 基于二维纳米材料的水处理功能膜研究进展[J]. 化工进展, 2021, 40(8): 4117-4126.

LI Zhouyan, DAI Ruobin, LI Yang, WANG Xueye, WANG Zhiwei. Research progress of functional membranes based on two-dimensional nanomaterials for water treatment[J]. Chemical Industry and Engineering Progress, 2021, 40(8): 4117-4126.

图/表 6

参考文献 59

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二维纳米材料	其他分离层组分	制备方法	分类	应用场景	最优条件	抗污染效果	参考文献
GO	激光诱导石墨烯（LIG），戊二醛	VAF自组装	导电膜	微（超）滤	3V，作为阳极	在混菌的错流过滤实验中，导电膜通量较普通超滤膜提升11%	［30］
Gr	PANI	PAF自组装	导电膜	正渗透	2V，作为阳极	在海藻酸钠污染实验中，污染速率降低40%~45%，通量恢复率提升20%~30%	［33］
rGO	PDVF，PDAAQ	相转化法	导电膜	膜生物反应器	1.0V·cm^-1，作为阴极	牛血清蛋白（BSA）的污染速率降低63.5%	［22］
GO	导电高分子聚吡咯（PPy）	气相聚合法	导电膜	膜生物反应器	1.0V·cm^-1，作为阴极	在酵母菌污染实验中，较对照组通量提升20%	［19］
GO	导电高分子聚吡咯（PPy）	气相聚合法	导电膜	膜生物反应器	2V·cm^-1，作为阴极，并投加群体感应淬灭细菌	在MBR中污染速率仅为其他对照组的34%~55%	［23］
Gr	基膜为镍基导电膜	化学气相沉积	导电膜	厌氧膜生物反应器	0.7V或0.9V，作为阴极，阴阳极间距约1.5cm的矩形反应器	运行50余天后，跨膜压力仅为0.10bar（0.7V）和0.05bar（0.9V），远低于管式反应器（0.7V）的0.46bar（1bar=10⁵Pa）	［48］

二维纳米材料	其他分离层组分	制备方法	分类	应用场景	最优条件	抗污染效果	参考文献
GO	激光诱导石墨烯（LIG），戊二醛	VAF自组装	导电膜	微（超）滤	3V，作为阳极	在混菌的错流过滤实验中，导电膜通量较普通超滤膜提升11%	［30］
Gr	PANI	PAF自组装	导电膜	正渗透	2V，作为阳极	在海藻酸钠污染实验中，污染速率降低40%~45%，通量恢复率提升20%~30%	［33］
rGO	PDVF，PDAAQ	相转化法	导电膜	膜生物反应器	1.0V·cm^-1，作为阴极	牛血清蛋白（BSA）的污染速率降低63.5%	［22］
GO	导电高分子聚吡咯（PPy）	气相聚合法	导电膜	膜生物反应器	1.0V·cm^-1，作为阴极	在酵母菌污染实验中，较对照组通量提升20%	［19］
GO	导电高分子聚吡咯（PPy）	气相聚合法	导电膜	膜生物反应器	2V·cm^-1，作为阴极，并投加群体感应淬灭细菌	在MBR中污染速率仅为其他对照组的34%~55%	［23］
Gr	基膜为镍基导电膜	化学气相沉积	导电膜	厌氧膜生物反应器	0.7V或0.9V，作为阴极，阴阳极间距约1.5cm的矩形反应器	运行50余天后，跨膜压力仅为0.10bar（0.7V）和0.05bar（0.9V），远低于管式反应器（0.7V）的0.46bar（1bar=10⁵Pa）	［48］

二维纳米材料	其他分离层组分	制备方法	分类	应用场景	实验参数	通量恢复效果	参考文献
rGO	PANI	PAF自组装	导电膜	微（超）滤	3~9V作为阳极进行清洗，阴阳极间距0.5cm	清洗实验中通量恢复率最高达到97%	［32］
rGO	有机主体为PES、PANI（HCSA）或PANI（DBSA）	相转化法	导电膜	微（超）滤	电压5V，清洗时间10min	在腐殖酸（HA）和BSA污染实验中，通量恢复率较超纯水清洗提升6%~8%，较普通PES膜提升48%~68%	［21］
rGO	二维TiO₂	溶剂热诱导组装	光催化膜	染料分离	可见光照射一定时间	通量恢复率约为95%	［47］
GO	一维TiO₂纳米棒	VAF自组装	光催化膜	染料分离	可见光照射24h，功率500W，照明距离35cm	3轮实验后，通量恢复率均大于83%	［43］
GO，g-C₃N₄	零维TiO₂	VAF自组装	光催化膜	油水分离	去离子水清洗20min，模拟光照1h	通量为普通GO膜的45倍，10轮油水分离试验后自清洁的通量恢复率仍高于95%	［36］
GO，g-C₃N₄	一维坡缕石（PG）、光催化剂Bi₂O₂CO₃	VAF自组装	光催化膜	油水分离	模拟光照射1h	通量为普通GO膜的46倍，自清洁的通量恢复率高于95%（最高接近100%）	［40］
g-C₃N₄	芬顿催化剂 Fe-POMs	氢键作用辅助的VAF自组装	光催化膜	染料分离	100mW·cm^-2模拟太阳光照，连续流实验中添加30mmol·L^-1 H₂O₂	5轮试验后，通量恢复率均接近100%；连续流实验中通量在12h内保持稳定	［46］

二维纳米材料	其他分离层组分	制备方法	分类	应用场景	实验参数	通量恢复效果	参考文献
rGO	PANI	PAF自组装	导电膜	微（超）滤	3~9V作为阳极进行清洗，阴阳极间距0.5cm	清洗实验中通量恢复率最高达到97%	［32］
rGO	有机主体为PES、PANI（HCSA）或PANI（DBSA）	相转化法	导电膜	微（超）滤	电压5V，清洗时间10min	在腐殖酸（HA）和BSA污染实验中，通量恢复率较超纯水清洗提升6%~8%，较普通PES膜提升48%~68%	［21］
rGO	二维TiO₂	溶剂热诱导组装	光催化膜	染料分离	可见光照射一定时间	通量恢复率约为95%	［47］
GO	一维TiO₂纳米棒	VAF自组装	光催化膜	染料分离	可见光照射24h，功率500W，照明距离35cm	3轮实验后，通量恢复率均大于83%	［43］
GO，g-C₃N₄	零维TiO₂	VAF自组装	光催化膜	油水分离	去离子水清洗20min，模拟光照1h	通量为普通GO膜的45倍，10轮油水分离试验后自清洁的通量恢复率仍高于95%	［36］
GO，g-C₃N₄	一维坡缕石（PG）、光催化剂Bi₂O₂CO₃	VAF自组装	光催化膜	油水分离	模拟光照射1h	通量为普通GO膜的46倍，自清洁的通量恢复率高于95%（最高接近100%）	［40］
g-C₃N₄	芬顿催化剂 Fe-POMs	氢键作用辅助的VAF自组装	光催化膜	染料分离	100mW·cm^-2模拟太阳光照，连续流实验中添加30mmol·L^-1 H₂O₂	5轮试验后，通量恢复率均接近100%；连续流实验中通量在12h内保持稳定	［46］

二维纳米材料	其他分离层组分	制备方法	分类	应用场景	关键参数	去除效果	参考文献
MoS₂	Fe（OH）₃作为模板，成膜后刻蚀掉	VAF自组装/ 模板刻蚀	其他功能膜	污染物降解	过一硫酸盐浓度为50ppm（1ppm=1mg/kg），pH为4，过滤性能为154L·m^-2·h^-1·bar^-1	接触时间为60.4ms，BPA（2ppm）的去除率大于90%	［45］
MoS₂	无	VAF自组装	其他功能膜	重金属去除	pH为6，反应时间为1天，MoS₂膜未经真空干燥	还原去除容量约为4000mg Ag/g MoS₂，远高于干燥后的MoS₂膜	［28］
Gr	TiO₂	溶胶凝胶法	导电膜/ 光催化膜	微（超）滤	pH为5.4，模拟太阳光照，4V作为阳极	30min光电协同对100mL罗丹明B（10mg·L^-1）的去除效率达97.8%，高于300min的光催化去除效率（87.6%）	［24］
GO	一维TiO₂纳米线，聚多巴胺	VAF自组装	光催化膜	油水/染料分离	可见光照射条件下，过滤性能为273L·m^-2·h^-1·bar^-1	对油水混合液中MB（10ppm）的去除率大于98%	［31］
GO	零维TiO₂、Co₃O₄	VAF自组装	光催化膜	油水分离	光源功率为250W	100mL刚果红/油水混合液，刚果红（20ppm）降解效率为82%	［37］
GO	零维纳米Ag、一维钛纳米管	VAF自组装	光催化膜	染料分离	可见光照射条件下，通量为34.7L·m^-2·h^-1	对MB（10mg·L^-1）的去除率大于65%，且通量约为无光照条件下的两倍	［38］
rGO	一维g-C₃N₄ 纳米管	VAF自组装	光催化膜	染料分离	300W可见光照射条件下，过滤性能为4.77L·m^-2·h^-1·bar^-1	对罗丹明B（5mg·L^-1）的去除率大于98%	［41］
GO， g-C₃N₄	一维CNTs	VAF自组装	光催化膜	污染物降解	可见光照射条件下，过滤性能为14.35L·m^-2·h^-1·bar^-1	罗丹明B和盐酸四环素去除率分别为98.31%、84.81%	［39］
GO	光Fenton催化剂：一维MOF （MIL-88A）	VAF自组装	光催化膜	染料分离	模拟太阳光104mW·cm^-2，10mmol·L^-1 H₂O₂	对50mL MB和BPA（10mg·L^-1）去除率分别为98.8%和97.3%	［42］