Development of antifouling reverse osmosis membranes for water treatment: A review Guo-dong Kang, Yi-ming Cao* Dalian National Laboratory for Clean Energy (DNL), Dalian Institute of Chemical Physics (DICP), Chinese Academy of Science (CAS), 457 Zhongshan Road, Dalian 116023, PR China article info Article history: Received 5 August 2011 Received in revised form 7 November 2011 Accepted 14 November 2011 Available online 23 November 2011 Keywords: Reverse osmosis Membrane fouling Antifouling property Surface modification abstract With the rapidly increasing demands on water resources, fresh water shortage has become an important issue affecting the economic and social development in many countries. As one of the main technologies for producing fresh water from saline water and other wastewater sources, reverse osmosis (RO) has been widely used so far. However, a major challenge facing widespread application of RO technology is membrane fouling, which results in reduced production capacity and increased operation costs. Therefore, many researches have been focused on enhancing the RO membrane resistance to fouling. This paper presents a review of developing antifouling RO membranes in recent years, including the selection of new starting monomers, improvement of interfacial polymerization process, surface modification of conventional RO membrane by physical and chemical methods as well as the hybrid organic/inorganic RO membrane. The review of research progress in this article may provide an insight for the development of antifouling RO membranes and extend the applications of RO technology in water treatment in the future. ª 2011 Elsevier Ltd. All rights reserved. Contents 1. Introduction ............................................................................................... 585 2. RO membrane fouling ...................................................................................... 586 3. Development of new RO material or improvement of interfacial polymerization process ......................... 587 3.1. Selection of new interfacial polymerization monomers .................................................. 587 3.2. Improvement of interfacial polymerization process ...................................................... 587 Abbreviations: AA, acrylic acid; ADMH, 3-allyl-5,5-dimethylhydantoin; AFM, atomic force microscope; AIBA, 2,2 0 -azobis(isobutyramidine) dihydrochloride; AMPS, 2-acrylamido-2- methylpropane-sulfonic acid; ATR-FTIR, attenuated total reflectance Fourier transform infrared spectroscopy; ATRP, atom transfer radical polymerization; BSA, bovine serum albumin; BTEC, 3,3 0 ,5,5 0 -biphenyl tetraacyl chloride; BTRC, 3,4 0 ,5-biphenyl triacyl chloride; DTAB, dodecyltrimethylammoniumbromide; HEA, 2-hydroxyethyl acrylate; ICIC, 5-isocyanato-isophthaloyl chloride; iCVD, initiated chemical vapor deposition; iLSMM, in situ hydrophilic surface modifying macromolecules; LFC, low fouling composite; MA, methacrylic acid; MDI, 4,4 0 -methylene bis(phenyl isocyanate); MDMH, 3-monomethylol-5,5-dimethylhydantoin; MF, microfiltration; MPD, m-phenylenediamine; NF, nanofiltration; PEG, poly(ethylene glycol); PEGA, poly(ethylene glycol) acrylate; PEGDA, poly(ethylene glycol) diacrylate; PEGDE, poly(ethylene glycol) diglycidyl ether; PEGMA, polyethyleneglycolmethacrylate; PEI, poly- ethyleneimine; PIP, piperazine; P(NIPAm-co-AAc), poly(N-isopropylacrylamide-co-acrylic acid); PVA, polyvinyl alcohol; RO, reverse osmosis; SEM, scanning electron microscope; SPEEK, sulfonated poly(ether ether ketone); SPM, 3-sulfopropyl methacrylate; TEM, trans- mission electron microscopy; TFC, thin-film composite; TFN, thin-film nanocomposite; TMC, trimesoyl chloride; UF, ultrafiltration; VSA, vinylsulfonic acid; XPS, X-ray photoelectron spectroscopy. * Corresponding author. Tel.: þ86 411 84379053; fax: þ86 411 84379329. E-mail address: [email protected](Y.-m. Cao). Available online at www.sciencedirect.com journal homepage: www.elsevier.com/locate/watres water research 46 (2012) 584 e600 0043-1354/$ e see front matter ª 2011 Elsevier Ltd. All rights reserved. doi:10.1016/j.watres.2011.11.041
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wat e r r e s e a r c h 4 6 ( 2 0 1 2 ) 5 8 4e6 0 0
wat e r r e s e a r c h 4 6 ( 2 0 1 2 ) 5 8 4e6 0 0 597
solution (Jeong et al., 2007). Nanoparticle dispersion was ob-
tained by ultrasonication for 1 h at room temperature imme-
diately prior to interfacial polymerization. Other fabrication
processes were same to the traditional method of TFC
membrane. The prepared zeoliteepolyamide membrane
surface showed enhanced hydrophilicity, more negative
charge and lower roughness, implying a strong potential use
as an antifouling membrane. Most recently, Fathizadeh et al.
performed a similar study (Fathizadeh et al., 2011). Never-
theless, they did not investigate the fouling resistance of
prepared hybrid RO membranes.
On the other hand, Rana et al. added 0.25 wt% of silver
salt (silver nitrate, or silver citrate hydrate or silver lactate)
into aqueous MPD phase instead of organic TMC phase to
prepare hybrid organic/inorganic RO membrane (Rana et al.,
2011). Meanwhile, the hydrophilic surface modifying
macromolecules (polyurethane end-capped with PEG) were
also added into aqueous phase containing MPD. In other
words, the authors combined the organic and inorganic
modifiers into RO membranes, optimizing the fouling resis-
tance. The results showed that silver salts incorporated in
the TFC membranes indeed improve the anti-biofouling
property.
At present, this method was also used in the development
of antifouling nanofiltration membranes (Lee et al., 2007;
Jadav and Singh, 2009). For example, Lee et al. prepared
polyamide/Ag nanocomposite membranes from in situ inter-
facial polymerization between aqueous MPD and organic TMC
together with 10 wt% of silver nanoparticles. The hybrid
membranes were shown to possess the dramatic anti-
biofouling effect on Pseudomonas. Moreover, most of the Ag
particles remained on the surface even after the performance
test, confirmed with SEM, XPS and AFM. It should be noted
that, however, besides of on membrane surface, some nano-
particles were also encapsulated within polyamide thin films,
reducing the antifouling or antimicrobial activities.
6. Conclusions and future perspectives
The development of antifouling is an important research
direction in RO technology for water treatment and has
attracted wide attention in recent years. In this paper, the
progress in this area is reviewed. The development methods
are related to the surface modification of conventional RO
membranes, improvement of interfacial polymerization
process and exploitation of new RO membranes.
Surface modification is an effective way to tailor
membrane surface properties, thus improving the fouling
resistant performance. Apart from the approaches and
hydrophilic modifiers mentioned above, some other methods
such as atom transfer radical polymerization (ATRP) tech-
nique and other modifiers such as zwitterionic charged
materials are also potential to develop antifouling RO
membranes. However, surface modification, either physical
method or chemical method, usually leads to the decline of
water flux. The trade-off of flux reduction and antifouling
property should be optimized and balanced. Moreover,
surface modification is conducted after the formation of RO
membrane, increasing the production difficulty and/or
operation cost. The method whereby the membrane fouling
resistance can be enhanced in situ (i.e., in preparation
process) is of particular interest from a practical point of view.
The addition of inorganic particles into polymeric
membranes is a new development direction in RO technology.
The hybrid organic/inorganic RO membranes show attractive
permeability characteristics, antifouling and self-cleaning
properties, and they are very promising in commercial use.
In fact, the nanocomposite RO membranes have been indus-
trialized in market at present (for example, http://www.
nanoh2o.com/) and may be extensively used in future.
Despite the achievements, there are still some issues or
challenges facing antifouling RO membranes. Firstly, many
development methods are confined to scientific research
currently due to high cost, complicated operation procedure
or difficulty in scaling up, and only few methods are ready for
commercial use. Secondly, the studies on long-term fouling
test should be paid further attention. The stability ofmodifiers
should be verified in actual application. In fact, the improve-
ment of antifouling property through some physical modifi-
cations, such as surface adsorption or even surface coating,
may be easily deteriorated in long-term operation due to the
loss of modifiers. Generally, the chemically covalent linkage
between membrane and modifiers is superior to physical
combination and has better practical utility. However, special
equipments or chemical reagents are usually needed in
chemical modification method. These will increase the
production cost or cause environmental pollution. Thirdly,
few studies are focused on the stability of surface modifiers in
cleaning operation. In fact, the cleaning is a necessary process
in RO membrane use. The acid, alkaline or other cleaning
environments may cause the degradation of modifiers, which
should be also considered in practical application.
Last, but not least, the fouling cannot be thoroughly pre-
vented even for antifouling membranes. There are no
membranes that are free from fouling under any circum-
stances (Rana and Matsuura, 2010). The selection and use of
RO membrane should be based on the foulants character in
feeding solution. Moreover, some other measures such as
module design optimization, proper pretreatment and effec-
tive membrane cleaning are also necessary.
Acknowledgments
Financial support from National Natural Science Foundation
of China (Grant No. 20906086) and Major State Basic Research
Development Program of China (Grant No. 2009CB623405) are
gratefully acknowledged.
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