High efficient removal of dyes from aqueous solution through nanofiltration using diethanolamine-modified polyamide thin-film composite membrane
Introduction
The removal of dyes from textile and dyeing wastewaters before discharging into the environment is of great importance, since the presence of dyes even at a very low concentration is highly visible and toxic to aquatic life through damaging the esthetic nature of water and reducing the photosynthetic activity of aquatic organisms [1], [2], [3], [4]. Technologies including physical removal, chemical treatment, and biological degradation have been developed to remove the dyes from wastewater. Of these technologies, biological degradation process using activated sludge cannot completely eliminate the color due to the biodegradable difficulty of many synthetic dyes [5], [6], physical processes including adsorption and coagulation/flocculation usually generate toxic sludge and are not suitable for large-scale applications [7], [8], advanced oxidation processes including chemical oxidation, catalytic degradation and electrochemical treatment are still quite costly for practical application [9], [10], [11], [12], [13], while physical membrane separation process employing nanofiltration (NF) membrane is promisingly attractive for the removal of dyes from wastewater for its production of high-quality effluent without the generation of sludge [14].
Therefore, many efforts have been devoted to remove dyes from wastewater by using different nanofiltration membranes. Qin et al. [15] treated dyeing wastewater for reuse by using three types of nanofiltration membranes designed as NE-70, Desal-5 and TS-40 and found that all the three studied membranes performed high efficiency of greater than99% for dye removal. Zuriaga-Agustí et al. [16] reported that the commercial available nanofiltration membrane NF270 could completely remove the color of the biologically treated simulated textile wastewater. Ellouze et al. [17] reported that the DK spiral wound nanofiltration membrane could achieve 100% color removal as the post treatment of coagulation-flocculation process in treatment of the industrial textile effluent. Ong et al. [18] treated textile wastewater using self-made polyamide-imide hollow fiber nanofiltration membrane through pilot-scale tests and found that the rejections to dyes reactive blue 19, reactive black 5 and reactive yellow 81 were all higher than 90%. More recently, Zhu et al. [19] fabricated a novel “loose” nanofiltration membrane by blending with chitosan–montmorillonite (CS–MMT) nanosheets via phase inversion method and found that the as-prepared membranes showed higher rejection for dyes and lower rejection for bivalent salts.
The aforementioned examples illustrate that nanofiltration membrane separation process can effectively remove dyes from wastewater and provide recovery of dyes and reuse of water. However, high energy consumption and sever membrane fouling are the two major obstacles that limit the extensive application of nanofiltration technology in treatment of textile and dyeing wastewaters [20], [21], [22]. So, it is essential to design and develop novel nanofiltration membranes with special surface properties that are more permeable to water and less prone to fouling.
The objective of this study was to improve the water permeability and fouling resistance of the state-of-art polyamide (PA) thin-film composite (TFC) nanofiltration membrane for high efficient removal of dyes from aqueous solution via surface modification, which has been proven to be a promising route to enhance membrane performance through modulating membrane surface properties [23], [24], [25]. Considering the fact that surface modifications could be performed with the freshly prepared interfacially synthesized PA-TFC nanofiltration membrane through using the residual acyl chloride groups, in this work, hydrophilic monomer diethanolamine (DEA) was adopted and grafted on polyamide nanofiltration membrane by a facile method of pouring the DEA-aqueous solution on the surface of the nascent (freshly prepared) polyamide membrane, which was fabricated through the interfacial polymerization of piperazine and trimesoyl chloride on the porous polysulfone support membrane. Compared with the approach of post amidation reaction between the residual acyl chloride groups and the amino groups of the grafting monomers such as poly (amidoamine) dendrimer and N-aminoethyl piperazine propane sulfonate that have been adopted by other researchers [26], [27], the reaction of monomer DEA with the residual acyl chloride group will avoid the formation of amide linkage (CONH) of poor chlorine stability [28]. The obtained PA-TFC membranes with and without DEA moisture were rigorously characterized in terms of physicochemical property, permeation performance, antifouling behaviors as well as dye removal performance.
Section snippets
Materials
Flat-sheet nonwoven-reinforced polysulfone (PSF) ultrafiltration support membrane with a molecular weight cut-off (MWCO) of around 80,000 g/mol and a pure water permeability of approximately 120 l/m2 h bar was supplied by Hangzhou Tianchuang Environmental Technology Co., Ltd., China. Monomers trimesoyl chloride (TMC, purity > 99.0%) and piperazine (PIP, purity > 99.5%) for interfacial polymerization were purchased from Sigma–Aldrich and used as received. Diethanolamine (DEA) was purchased from
Physicochemical properties of the DEA-modified PA-TFC membrane
ATR-FTIR and XPS were adopted to detect the chemical structure and composition of the active layer of the DEA-modified PA-TFC membrane. The ATR-FTIR spectra of the PA-TFC membranes with and without DEA moisture are shown in Fig. 3. It can be found that no new peak appears in the ATR-FTIR spectrum of the DEA-modified membrane compared with that of the traditional PA-TFC membrane with no DEA moisture, and the DEA-modified membrane shows a higher ratio of the heights of the characteristic peaks of
Conclusions
The removal of dyes from aqueous solution through nanofiltration using tailor-fabricated DEA-modified polyamide thin-film composite membrane has been investigated. The covalent attachment of DEA molecules on the surface of the traditional polyamide thin-film composite membrane was found to make membrane surface more hydrophilic and less negatively charged under neutral pH and to have no influence on the thickness and compactness of the active layer. The DEA-modified membrane exhibited the same
Acknowledgements
The authors gratefully acknowledge the financial supports of the National Natural Science Foundation of China (NNSFC) (Grant Nos. 21476213 and 21676256) and the 521 personnel training plan of Zhejiang Sci-Tech University.
References (46)
- et al.
Remediation of dyes in textile effluent: a critical review on current treatment technologies with a proposed alternative
Bioresour. Technol.
(2001) - et al.
Aquatic toxicity of dyes before and after photo-Fenton treatment
J. Hazard. Mater.
(2014) - et al.
Combined anaerobic–ozonation process for treatment of textile wastewater: removal of acute toxicity and mutagenicity
J. Hazard. Mater.
(2015) - et al.
Anaerobic/aerobic treatment of a simulated textile wastewater
Sep. Purif. Technol.
(2008) - et al.
Sequential chemical–biological processes for the treatment of industrial wastewaters: review of recent progresses and critical assessment
J. Hazard. Mater.
(2014) Treatment of paint manufacturing wastewater by electrocoagulation
Desalination
(2012)- et al.
Chemical Oxygen Demand (COD) reduction of a reactive dye wastewater using H2O2/pyridine/Cu(II) system
Desalination
(2011) - et al.
Recent developments of zinc oxide based photocatalyst in water treatment technology: a review
Water Res.
(2016) - et al.
Comparative decolorization of dyes in textile wastewater using biological and chemical treatment
Sep. Purif. Technol.
(2015) Electrochemical technologies in wastewater treatment
Sep. Purif. Technol.
(2004)
Nanofiltration for recovering wastewater from a specific dyeing facility
Sep. Purif. Technol.
Sequencing batch reactor technology coupled with nanofiltration for textile wastewater reclamation
Chem. Eng. J.
Enhancement of textile wastewater treatment process using nanofiltration
Desalination
Nanofiltration hollow fiber membranes for textile wastewater treatment: lab-scale and pilot-scale studies
Chem. Eng. Sci.
Fabrication of a novel “loose” nanofiltration membrane by facile blending with Chitosan-Montmorillonite nanosheets for dyes purification
Chem. Eng. J.
Drawbacks of applying nanofiltration and how to avoid them: a review
Sep. Purif. Technol.
Polymeric nanofiltration membranes for textile dye wastewater treatment: preparation, performance evaluation, transport modelling, and fouling control – a review
Desalination
Fouling of nanofiltration membranes by dyes during brine recovery from textile dye bath wastewater
Chem. Eng. J.
A review on nanofiltration membrane fabrication and modification using polyelectrolytes: effective ways to develop membrane selective barriers and rejection capability
Adv. Colloid Interface
Surface-modified reverse osmosis membranes applying a copolymer film to reduce adhesion of bacteria as a strategy for biofouling control
Sep. Purif. Technol.
Improvement of antibiofouling performance of a reverse osmosis membrane through biocide release and adhesion resistance
Sep. Purif. Technol.
Poly(amidoamine) dendrimer (PAMAM) grafted on thin film composite (TFC) nanofiltration (NF) hollow fiber membranes for heavy metal removal
J. Membr. Sci.
A novel route for surface zwitterionic functionalization of polyamide nanofiltration membranes with improved performance
J. Membr. Sci.
Cited by (210)
Integrating binary organic phosphonic acid into nanofiltration membrane for high precision separation of mono-/divalent anions
2024, Separation and Purification TechnologyConstruction of PDA-PEI/ZIF-L@PE tight ultra-filtration (TUF) membranes on porous polyethylene (PE) substrates for efficient dye/salt separation
2024, Journal of Hazardous MaterialsSeparation of microbial and organic pollutants from water using low-pressure tailor-made membranes
2024, Advances in Drinking Water Purification: Small Systems and Emerging Issues