water research 43 (2009) 14891512

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Review

Recent advances in membrane bioreactors (MBRs): Membrane fouling and membrane material
Fangang Menga,c,*, So-Ryong Chaeb, Anja Drewsc, Matthias Kraumec, Hang-Sik Shind, Fenglin Yanga
Key Laboratory of Industrial Ecology and Environmental Engineering, MOE, School of Environmental and Biological Science and Technology, Dalian University of Technology, Dalian 116024, PR China b Department of Civil and Environmental Engineering, School of Engineering, Duke University, Durham, NC 27708, USA c Chair of Chemical Engineering, Technische Universita t Berlin, Str. des 17. Juni 135, MA 5-7, 10623 Berlin, Germany d Department of Civil and Environmental Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, South Korea
a

article info
Article history: Received 7 April 2008 Received in revised form 19 December 2008 Accepted 22 December 2008 Published online 3 January 2009 Keywords: Membrane bioreactor (MBR) Membrane fouling Extracellular polymeric substances (EPS) Soluble microbial products (SMP) Membrane modication

abstract
Membrane bioreactors (MBRs) have been actively employed for municipal and industrial wastewater treatments. So far, membrane fouling and the high cost of membranes are main obstacles for wider application of MBRs. Over the past few years, considerable investigations have been performed to understand MBR fouling in detail and to develop high-ux or low-cost membranes. This review attempted to address the recent and current developments in MBRs on the basis of reported literature in order to provide more detailed information about MBRs. In this paper, the fouling behaviour, fouling factors and fouling control strategies were discussed. Recent developments in membrane materials including low-cost lters, membrane modication and dynamic membranes were also reviewed. Lastly, the future trends in membrane fouling research and membrane material development in the coming years were addressed. 2009 Elsevier Ltd. All rights reserved.

Abbreviations: AFM, atomic force microscopy; AGMBR, aerobic granular sludge membrane bioreactor; ANN, articial neural network; BAC, biologically activated carbon; BAP, biomass-associated products; BOD, biological oxygen demand; CFD, computational uid dynamics; CLSM, confocal laser scanning microscopy; COD, chemical oxygen demand; CST, capillary suction time; DGGE, denaturing gradient gel electrophoresis; DO, dissolved oxygen; DOC, dissolved organic carbon; DON, dissolved organic nitrogen; DOTM, direct observation through membrane; EPS, extracellular polymeric substance; F/M, food to microorganism ratio; FISH, uorescence in situ hybridization; FTIR, Fourier transform infrared spectroscopy; HP-SEC, high performance size exclusion chromatography; HRT, hydraulic retention time; MBR, membrane bioreactor; MF, microltration; MFE, membrane ux enhancer; MFR, membrane fouling reducer; MLSS, mixed liquid suspended solid; NF, nanoltration; NMR, nuclear magnetic resonance; OLR, organic loading rate; PAC, powdered activated carbon; PAN, polyacrylonitrile; PCR, polymerase chain reaction; PE, polyethylene; PES, polyethersulfone; PFS, polymeric ferric sulfate; POEM, polyoxyethylene methacrylated; PPHFMM, polypropylene hollow ber microporous membrane; PVDF, polyvinylidene uoride; RO, reverse osmosis; SEM, scanning electron microscopy; SMP, soluble microbial products; SRF, sludge resistance to ltration; SRT, solid retention time; TFC, thin lm composite; TMP, transmembrane pressure; UAP, substrate-utilisation-associated products; UF, ultraltration; VSS, volatile suspended solid. * Corresponding author. Key Laboratory of Industrial Ecology and Environmental Engineering, MOE, School of Environmental and Biological Science and Technology, Dalian University of Technology, Dalian 116024, PR China. Tel.: 86 411 84706172. E-mail address: fgmeng80@126.com (F. Meng). 0043-1354/$ see front matter 2009 Elsevier Ltd. All rights reserved. doi:10.1016/j.watres.2008.12.044

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Contents
1. 2. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Fundamentals of membrane fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.1. Characteristics of membrane fouling and its importance in MBRs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2. Classification of membrane fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.1. Removable and irremovable fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.1.1. Definition of removable and irremovable fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.1.2. Formation of the cake layer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.1.3. Irremovable fouling in MBRs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.2. Biofouling, organic fouling, and inorganic fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.2.1. Biofouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.2.2. Organic fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2.2.2.3. Inorganic fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Fouling factors and control strategies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1. Bound EPS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1.1. Definition of bound EPS and SMP . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1.2. Effect of bound EPS on membrane fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1.3. Behaviour and control of bound EPS in MBRs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2. SMP . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2.1. Effect of SMP on membrane fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2.2. Behaviour and control of SMP in MBRs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2.2.1. Control of SMP via adjustment of operation conditions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2.2.2. Control of SMP via addition of adsorbents/coagulants . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3. Hydrodynamic conditions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3.1. Effect of hydrodynamic conditions on membrane fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.3.2. Favorable hydrodynamic conditions mitigating membrane fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.4. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Developments of membranes/filters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.1. Influence of membrane characteristics on MBR performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.2. Application of low-cost filters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.3. Membrane modification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4.4. Dynamic membranes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Conclusions and perspectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

3.

4.

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1.

Introduction

MBRs are being increasingly used for wastewater treatment that requires excellent efuent quality, e.g., water reuse or water recycling (Judd, 2006, 2008; Liao et al., 2006; Yang et al., 2006; Wang et al., 2008a). MBRs allow high concentrations of mixed liquor suspended solids (MLSS) and low production of excess sludge, enable high removal efciency of biological oxygen demand (BOD) and chemical oxygen demand (COD), and water reclamation. However, membrane fouling is a major obstacle to the wide application of MBRs. Additionally, large-scale use of MBRs in wastewater treatment will require a signicant decrease in price of the membranes. During the last few years, Chang et al. (2002a) and Le-Clech et al. (2006) reviewed MBR fouling by focusing on almost all the fouling factors; namely, they provided a very comprehensive review on sludge characteristics, operational parameters, membrane materials and feedwater characteristics. In recent years, a considerable number of papers were published, e.g., the annual publication reached nearly 400 in 2006 and 2007 (see Fig. 1). To date we are still confused with MBR fouling, even though numerous investigations have been performed. In fact, the complex nature of membrane foulants and

activated sludge is the main cause that puzzles us. Furthermore, these investigations were of different focus and therefore, it is necessary to summarize and compare the results obtained in recent years. To complement the current knowledge on MBR fouling, this review paper was mainly focused on two issues:

Annual publications on MBR fouling (Google scholar)

1000

Number of publications

100

10

1 1994

1996

1998

2000

2002

2004

2006

2008

Year
Fig. 1 The diagram showing the annual publication on MBR fouling.

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Biomass-related aspects

MBR fouling (Foulants) Determine fouling

Activated sludge

Control fouling

Modify sludge

Aeration, Cleaning Operation conditions

SRT, HRT, F/M, DO, OLR

Fig. 2 Schematic illustration showing the fouling affecting factors and controlling approaches.

clogging and sludge cake deposition on membranes which is usually the predominant fouling component (Lee et al., 2001). Membrane fouling results in a reduction of permeate ux or an increase of transmembrane pressure (TMP) depending on the operation mode. With respect to MBRs, membrane fouling occurs due to the following mechanisms: (1) adsorption of solutes or colloids within/on membranes; (2) deposition of sludge ocs onto the membrane surface; (3) formation of a cake layer on the membrane surface; (4) detachment of foulants attributed mainly to shear forces; (5) the spatial and temporal changes of the foulant composition during the long-term operation (e.g., the change of bacteria community and biopolymer components in the cake layer). In other words, the membrane fouling can be dened as the undesirable deposition and accumulation of microorganisms, colloids, solutes, and cell debris within/on membranes. Given the complex nature of the activated sludge, it is not surprising that the fouling behaviour in MBRs is more complicated than that in most membrane applications. Generally, as shown in Fig. 4, a three stage fouling history might be proposed (Cho and Fane, 2002; Zhang et al., 2006a): - Stage 1: an initial short-term rapid rise in TMP; - Stage 2: a long-term weak rise in TMP; - Stage 3: a sharp increase in dTMP/dt, also known as TMP jump (Cho and Fane, 2002). Fig. 4 shows the schematic illustration of the occurrence of TMP jump. The TMP jump is believed to be the consequence of severe membrane fouling. Cho and Fane (2002) attributed the TMP jump to the changes in the local ux due to fouling eventually causing local uxes to be higher than the critical ux. Latterly, Zhang et al. (2006a) reported that the sudden jump was possibly not only due to the local ux effect, but also caused by sudden changes of the biolm or cake layer structure. Due to oxygen transfer limitation, the bacteria in the inner biolms tend to die and release more extracellular polymeric substances (EPS). A more recent investigation also conrmed that the sudden jump of TMP was closely related to the sudden increase in the concentration of EPS at the bottom of cake layer, which might be attributed to the death of bacteria in the inner of cake layer (Hwang et al., 2008). The occurrence of the TMP jump also depends on operating conditions. Zhang et al. (2006a) observed that an abrupt TMP jump of over 10 kPa was observed at 24 and 48 h for the uxes of 30 and 20 L/(m2 h), respectively, in a lab-scale MBR which was used to treat synthetic wastewater. However, there was no TMP jump during the 280 h operation at 10 L/(m2 h). Pollice et al. (2005) reported that the TMP jump was more frequently observed in small-scale experiments. It should be borne in mind that fouling rates measured in lab-scale are

fundamentals of membrane fouling (see Section 2) and sludge characteristics (see Section 3). The operating parameters such as SRT, HRT, dissolved oxygen (DO) and food to microorganism ratio (F/M) have no direct effect on membrane fouling; but they determine the sludge characteristics and, the optimisation of them can modify activated sludge (see Fig. 2). Therefore, to nd out the effective approaches (e.g., suitable operating parameters) for the modication of activated sludge, the inuence of operating parameters on sludge characteristics was analysed in this review paper. In addition, this paper also updated recent challenges for characterisation and control of membrane fouling by incorporating some new ndings such as the inuence of lamentous bulking on MBR fouling and the use of computational uid dynamics (CFD). Lastly, the development of new membrane/lter materials to overcome current problems related to membrane cost and membrane fouling was discussed.

2.

Fundamentals of membrane fouling

2.1. Characteristics of membrane fouling and its importance in MBRs

Membrane fouling is a major obstacle that hinders faster commercialisation of MBRs. As shown in Fig. 3, membrane fouling in MBRs can be attributed to both membrane pore

b
Sludge particles Colloids Solutes

Fig. 3 Membrane fouling process in MBRs: (a) pore blocking and (b) cake layer.

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TMP Jump

Filtration time
Fig. 4 Schematic illustration of the occurrence of TMP jump.

removable fouling, irremovable fouling and irreversible fouling. As shown in Fig. 5, the removable fouling can be easily eliminated by implementation of physical cleaning (e.g., backwashing) while the irremovable fouling needs chemical cleaning to be eliminated. The removable fouling and reversible fouling are the same. The removable fouling is caused by loosely attached foulants; however, irremovable fouling is caused by pore blocking and strongly attached foulants during ltration. The irreversible fouling is a permanent fouling which cannot be removed by any approaches. In general, removable fouling is attributed to the formation of cake layer, and the irremovable fouling is attributed to pore blocking.

TMP

inappropriate to describe long-term full-scale operation due to distinct and inherent differences between them (Kraume et al., 2009). From these investigations it can be concluded that the interactions between TMP jump and these operating parameters are very complex, and TMP jump occurs inevitably during long-term operation of MBRs. Thus, the overall goal of fouling control is to retard the occurrence of the TMP jump via modifying sludge characteristics or decreasing membrane ux (e.g., operation below critical ux). In MBRs, the prediction or measurement of fouling resistance is signicant for the understanding of fouling extent, or for the optimisation of operating conditions. Furthermore, the knowledge of the ltration mechanisms can help to nd an appropriate method to avoid fouling. Some empirical models have also been proposed, which aim at expressing the relation between sludge characteristics or operating conditions and membrane fouling. Table 1 shows the expressions developed to describe membrane ux or membrane fouling resistance in MBRs. These empirical models are helpful for the understanding and mitigation of membrane fouling in MBRs.

2.2. 2.2.1.

Classication of membrane fouling Removable and irremovable fouling

2.2.1.1. Denition of removable and irremovable fouling.

Membrane fouling is a very complicated phenomenon and results from multiple causes. Particle sizes of sludge ocs, colloids and solutes in mixed liquor may strongly affect fouling mechanisms in a membrane ltration system. If foulants are comparable with the membrane pores (i.e., colloids), or smaller than the membrane pores (i.e., solutes), adsorption on pore wall and pore blocking may occur. However, if foulants (i.e., sludge ocs and colloids) are much larger than the membrane pores, they tend to form a cake layer on the membrane surface. By now, the concepts of reversible fouling and irreversible fouling are confusing because of different denitions proposed in publications. Generally, the irreversible fouling should be dened as the fouling that cannot be removed by any methods including chemical cleaning. But, some previous studies dened the irreversible fouling as the fouling that can be removed by chemical cleaning but cannot be removed by physical cleaning. Here, we dene three types of fouling:

2.2.1.2. Formation of the cake layer. In many cases, cake layer formation linked with removable fouling was considered as the major contributor to membrane fouling in MBRs. Lee et al. (2001) reported that the ltration resistances included membrane resistance (12%), cake resistance (80%), blocking and irremovable fouling resistance (8%), indicating that the formation of cake layer is the main cause leading to membrane fouling. Table 2 shows the relevant reports about the importance of cake layer formation on membrane fouling. Recently, a large number of scientic investigations have been performed in order to gain a better understanding of cake layer formation and cake layer morphology. Chu and Li (2005) reported that the cake layer was not uniformly distributed on the entire surface of all of the membrane bers. The membranes were covered partially by a static sludge cake that could not be removed by the shear force due to aeration, and partially by a thin sludge lm that was frequently washed away by aeration turbulence. The ltration resistances of the sludge cake and thin sludge lm were 308 1011 and 32.5 1011 m1, respectively. They also pointed out that the deposited biopolymers allow easier and faster bacterial adhesion. In addition, the EPS holds the ocs more tightly on the membrane and increases the difculty of cake removal by aeration turbulence. Jeison and van Lier (2007) performed a study on a lab-scale anaerobic submerged membrane bioreactor (AnMBR) for over 200 days, and observed that cake formation was removable on a short-term basis, however, cake consolidation was observed when a long-term operation was performed at a ux close to the critical ux. The consolidated cake could not be removed by the back-ush cycles, and required an external physical cleaning procedure. At the same time, Di Bella et al. (2007) found that the cake in an aerobic MBR had a mainly removal nature. These investigations suggest that the cake layer formed with aerobic sludge and anaerobic sludge might have different removability. A cake layer can be described as a porous media with a complex system of interconnected inter-particle voids. Yang et al. (2007) simulated the intra-layer ow eld by using the three-dimensional volumetric grid model and confocal laser scanning microscopy (CLSM) analysis, and observed that there was a very complex ow pattern in the fouling layer. Because of the inter-connectivity of the neighboring pores, the ow direction may even be the reverse of that of the pressure gradient (dP/dx). Recently, multiphoton microscopy, which provides in situ 3D characterisation, was employed to characterise protein or yeast fouling, and a combination of 3D images and resistance data could be used to identify the

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Table 1 Expressions developed to describe membrane ux or membrane fouling resistance (modied after Judd and Jefferson, 2003). Application Expressiona Remarks
2

Ref.
(Shimizu et al., 1993; Chang et al., 2001; Chang and Kim, 2005) (Ishiguro et al., 1994) (Sato and Ishii, 1991) (Krauth and Staab, 1993)

J is membrane ux (L/m h), DP is TMP, CMLSS is the biomass concentration (mg/L), m is sludge viscosity (mPa s), a is specic cake resistance (m/kg). DCDOC is the differential DOC concentration between the Concentration J a b logDCDOC activated sludge and the permeate (mg/L). polarisation DP  Cross-ow J  CMLSS is sludge concentration (mg/L), CCOD is COD value :926 1:37 0:326 m Rm 843DPC0 MBR (mg/L), m is sludge viscosity (mPa s). MLSS CCOD m   MLSS is sludge concentration (kg/m3), MLVSS is volatile Cross-ow kReCMLSS CMLVSS J J0 exp sludge concentration (kg/m3), k is a constant related with MBR CMLVSS TMP, Re is Reynolds number. J0 is the initial membrane ux (L/m2 h). The accumulation, detachment and consolidation of EPS Submerged Rt Rm am on the membranes were considered. m is EPS density on MBR the membrane surface (kg/m2). Vp XTSS The activated sludge model No. 1 (ASM1) is used to Submerged Rt Rm am m km A describe membrane fouling. Where a is specic resistance MBR of accumulated mass (m/kg), m is accumulated mass on the membranes (kg/m2), A is membrane area (m2), Vp is permeate volume (m3), XTSS is total suspended solids, km is efciency of cross-ow velocity, ranging from 0 to 1. 0:532 3:05 Submerged K 8:93 107 CMLSS J0:376 Ua K is the increasing rate of ltration resistance (1/(m h)), X is MBR sludge concentration (mg/L), J is membrane ux (L/m2 h), ULr is observed cross-ow velocity of the tap water in the membrane zone (m/s). 5 Rf 2:25 expMLSS 9 10 0:111EPS Rf is the fouling resistance after 4 hours ltration with Submerged 2 1:99 10 PSD 3:20 a constant TMP of 3.97 kPa, EPS is the bound extracellular MBR polymeric substances (mg/g-MLSS), PSD is mean particle size (mm).

DP Classical cake J mRm aCMLSS ltration

(Nagaoka et al., 1998)

(Lee et al., 2002)

(Liu et al., 2003)

(Meng et al., 2006b)

dominant fouling mechanism (Hughes et al., 2006, 2007). The multiphoton microscopy might provide a potential method to study MBR fouling, especially for the study of soluble microbial product (SMP) fouling.

2.2.1.3. Irremovable fouling in MBRs. Although most of the

recent research activities are focused on the fundamental understanding of the cake layer, the investigation and control of irremovable membrane fouling is of great importance for long-term and sustainable operation of MBRs. During initial ltration, colloids, solutes and microbial cells pass through and precipitate inside the membrane pores. But, during the long-term operation of MBRs, the deposited cells multiply and yield EPS, which clog the pores and form a strongly attached fouling layer. At the same time, some inorganic substances might progressively precipitate onto the membranes or into the membrane pores (see Section 2.2.2). The occurrence of MBR fouling is a very complex process. Thus, how to predict and control fouling is of great signicance for MBR operation. Operation below the critical ux is an effective approach to avoid severe fouling including removal and irremovable fouling within a given ltration system. Field et al. (1995) introduced critical ux concept, operation below the critical ux concept is called sub-critical ux or non-fouling operation and is expected to lead to little irremovable fouling. For a short-term membrane ltration, when the permeate ux is set below the critical ux, the TMP remains stable and fouling was removable. In contrast, when it exceeds the critical ux, the TMP increases and might lead to a TMP jump. As a matter of fact, for a long-term operation of MBRs, irremovable fouling

can occur even if they are operated below the critical ux. Ognier et al. (2004) reported that despite the initial choice of sub-critical ux ltration conditions, gradual fouling was seen to develop which, after long periods of operation without intermediary membrane regeneration, proved to be hydraulically irremovable. The critical ux value depends on membrane characteristics, operating conditions (i.e., aeration intensity, temperature), and sludge characteristics. Further discussion of critical ux can be found in recent review articles (Pollice et al., 2005; Bacchin et al., 2006). The concept of critical ux has been popularly used in the study of MBR fouling (Guglielmi et al., 2007b; Lebegue et al., 2008; Wang et al., 2008b). However, most of the investigations on the determination of critical ux are based on ex-situ measuring, which cannot offer the real fouling propensity. Recently, an in situ method was developed by de la Torre et al. (2008), which can provide more reliable information about critical ux than ex-situ methods. Huyskens et al. (2008) developed an on-line measuring method, which was used to evaluate the removable and irremovable fouling propensity of MBR mixed liquor in a reproducible way. These studies imply that it is possible to develop on-line or in situ method to determine critical ux or removable/irremovable fouling. It is also of high interest to develop a unied measuring method or apparatus. Since irremovable fouling plays an important role in longterm operation of MBRs, sometimes chemical cleaning is required to maintain MBR operation. But, chemical cleaning for the elimination of irremovable fouling should be limited to a minimum frequency because repeated chemical cleaning may shorten the membrane lifetime and disposal of spent

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New membrane

Irreversible fouling

Initial filtration Chemical cleaning

Long-term filtration

Physical cleaning

Removable fouling irremovable fouling

and

Irremovable fouling Colloids Solutes

Sludge flocs

Fig. 5 Schematic illustration of the formation and removal of removable and irremovable fouling in MBRs.

chemical agents causes environmental problem (Yamamura et al., 2007).

2.2.2.

Biofouling, organic fouling, and inorganic fouling

2.2.2.1. Biofouling. From the viewpoint of fouling components, the fouling in MBRs can be classied into three major categories: biofouling, organic fouling, and inorganic fouling. A fundamental understanding of the formation of membrane

Table 2 Role of cake formation in membrane fouling. Feedwater

Synthetic wastewater

Effect of cake layer on membrane fouling

- Cake formation was entirely governing the applicable ux

Ref.
(Jeison and van Lier, 2007) (Ramesh et al., 2007)

Municipal wastewater

- The resistance of cake layer accounts for 9598% of the total ltration resistances (sludge ltration) - The specic ltration resistance of cake sludge was about 258 times higher than that of bulk sludge - The cake resistance was the dominant resistance and the bulking sludge could cause a severe cake fouling - Cake layer resistance was the major resistance - At high permeate ux, cake resistance (Rc) prevailed internal fouling resistance (Rf). At low permeate ux, Rf affect more greatly than Rc

(Wang et al., 2007) (Meng and Yang, 2007c)

(Chu and Li, 2006) (Shin et al., 2005)

Agricultural wastewater

foulants will help us to propose more effective approaches for fouling control. Biofouling refers to the deposition, growth and metabolism of bacteria cells or ocs on the membranes, which has aroused a signicant concern in membrane ltration processes (Pang et al., 2005; Wang et al., 2005). For a low pressure membrane such as microltration and ultraltration for treating wastewater, biofouling is a major problem because most foulants (microbial ocs) in MBRs are much larger than the membrane pore size. Biofouling may start with the deposition of individual cell or cell cluster on the membrane surface, after which the cells multiply and form a biocake. Many researchers suggest that SMP and EPS secreted by bacteria also play important roles in the formation of biological foulants and cake layer on membrane surfaces (Flemming et al., 1997; Liao et al., 2004; Ramesh et al., 2007). The deposition of bacteria cells can be visualised by techniques such as scanning electron microscopy (SEM), CLSM, atomic force microscopy (AFM), and direct observation through the membrane (DOTM). DOTM and CLSM have been extensively used to characterise membrane biofouling (Li et al., 2003; Jin et al., 2006; Yun et al., 2006; Zhang et al., 2006a; Hwang et al., 2007; Lee et al., 2007). The DOTM approach was originally developed by Fanes group at the University of New South Wales to record the deposition behaviour in simple cases of latex particles and ocs (Li et al., 2003; Zhang et al., 2006a). Zhang et al. (2006a) used a DOTM to observe the interactions between the bioocs and the membrane surface. The images showed that the bioocs could move across the membrane surface by rolling and sliding. More recently, CLSM has become a powerful approach for characterisation of membrane biofouling, which can not only identify the deposited cell, but also present the 3D structure of the fouling layer. Ng et al. (2006b) applied CLSM to visualise the bacterial distribution on the membrane surface, and found that bacteria were widely present on the fouled membrane. The combination of CLSM and image analysis can visualise or quantify the architecture of bio-cake layer (Lee et al., 2008). Yun et al. (2006) characterised the biolm structure and analysed its effect on membrane permeability in MBR for dye wastewater treatment. They found that membrane lterability was closely associated with the structural parameters of the biolms (i.e., porosity, biovolume). The visualisation of biofouling using these techniques is helpful for understanding of the oc/cell deposition process and the microstructure or architecture of the cake layer. In addition, a few investigations have been performed to study the microbial community structures and microbial colonisation on the membranes in MBRs (Chen et al., 2004; Jinhua et al., 2006; Zhang et al., 2006c; Miura et al., 2007). The microbial community structures can be investigated using microbiology methods such as polymerase chain reaction denaturing gradient gel electrophoresis (PCRDGGE) and Fluorescence In Situ Hybridization (FISH). Zhang et al. (2006c) reported that the microbial communities on membrane surfaces could be very different from the ones in the suspended biomass. They provided a list of bacteria that might be the pioneers of surface colonisation on membranes. Miura et al. (2007) studied the microbial communities in a full-scale submerged MBR used to treat real municipal wastewater delivered from the primary sedimentation basin of a municipal wastewater treatment

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facility over 3 months. They also reported that the microbial communities on membrane surfaces were quite different from those in the suspended biomass. In this study, their FISH and 16S rRNA gene sequence analyses revealed that a specic phylogenetic group of bacteria, the Betaproteobacteria, probably played a major role in development of the mature biolms, which led to severe irremovable membrane fouling. Jinhua et al. (2006) reported that g-Proteobacteria more selectively adhered and grew on membranes than other microorganisms, and the deposited cells have higher surface hydrophobicity than the suspended sludge. The high shear stress induced by aeration can select the deposition of cells. Some cells can be detached easily by the shear stress, but other ones still adhere to membrane surface tightly. The selective deposition of the cell relies on the afnity of cells to membranes. And, due to the anoxic condition in the cake layer, the temporal change of microbial community structure would take place. We can see that some of the bacteria in the sludge should play an important role in membrane biofouling. The fundamental understanding of deposition behaviour of bioocs/cells and mechanisms of cell attachment in MBRs will be crucial for the development of appropriate biofouling control strategies in the future.

fouling layer appeared to be made of protein-like substances, organic colloids and humic-like substances. A study by Teychene et al. (2008) showed that the fouling layer was mostly governed by the deposition of soluble compounds whereas the impact of the colloidal fraction (poorly present in the supernatant) was less; and the results of HP-SEC and uorescence analyses revealed the important role of protein-like substances (polypeptides) in MBR fouling. But, an early study by Rosenberger et al. (2006) demonstrated that polysaccharides and other non-settleable organic matter with a molecular weight larger than 120,000 Da were found to impact on membrane fouling. Additionally, high polysaccharide concentrations in sludge supernatant corresponded to high fouling rates. These studies conrm that SMP or EPS is the origin of organic fouling, and it plays signicant roles in the development of MBR fouling. In addition to the molecular size, the deposition of SMP or EPS on membranes strongly depends on its afnity with membranes.

2.2.2.2. Organic fouling. Organic fouling in MBRs refers to the deposition of biopolymers (i.e., proteins and polysaccharides) on the membranes. Due to the small size, the biopolymers can be deposited onto the membranes more readily due to the permeate ow, but they have lower back transport velocity due to lift forces in comparison to large particles (e.g., colloids and sludge ocs). Recently, in order to provide a unique insight into the composition (protein and carbohydrate), Metzger et al. (2007) have performed a more detailed study to characterise deposited biopolymers in MBRs. After membrane ltration, the fouling layers were fractionated into upper layer, intermediate layer and lower layer by using rinsing, backwashing and chemical cleaning. The results showed that the upper fouling layer was composed of a porous, loosely bound cake layer with a similar composition to the sludge ocs. The intermediate fouling layer was contributed equally by SMP and bacteria aggregates, and had a high concentration of polysaccharides. The lower layer, representing the irremovable fouling fraction and predominated by SMP, had a relative higher concentration of bound proteins. This study revealed the spatial distribution of biopolymers on the membrane surface. In order to gure out the detailed information on the deposited biopolymers, identication of these matters is indispensable. Fourier transform infrared (FTIR) spectroscopy, solid state 13C-nuclear magnetic resonance (NMR) spectroscopy and high performance size exclusion chromatography (HP-SEC) are powerful analytical tools for investigation of the organic fouling. They have been proven as effective approaches for identication and characterisation of organic fouling in MBRs. Through the FTIR spectra, the major components of the biopolymers were identied as proteins and polysaccharides (Zhou et al., 2007). 13C-NMR analysis by Kimura et al. (2005) also suggested that the foulants were rich in proteins and polysaccharides, however, different F/M ratios would change the nature of the foulants. The HP-SEC and uorescence analyses can help to conclude that membrane

2.2.2.3. Inorganic fouling. In general, membrane fouling in MBRs is mainly governed by biofouling and organic fouling rather than by inorganic fouling, although all of them take place simultaneously during membrane ltration of activated sludge. Up to now, thereby, most of the researchers attributed membrane fouling to the deposition of bacteria cells and biopolymers; the inorganic fouling in MBRs has been mentioned by only a few papers. Kang et al. (2002) investigated the ltration characteristics of organic and inorganic membranes in a membrane-coupled anaerobic bioreactor, in which a thick cake layer composed of biomass and struvite (MgNH4PO4$H2O) formed on the membranes, especially on the inorganic membrane. Ognier et al. (2002) pointed out there was severe CaCO3 fouling in a pilot MBR with a ceramic ultraltration membrane module. In this study, the synthetic wastewater was prepared with hard tap water (concentrations of Ca2 and Mg2 are 120 mg/L and 8 mg/L, respectively). They found that the high alkalinity of the activated sludge (pH 89) could cause the precipitation of CaCO3. The investigations by Kang et al. (2002) and Ognier et al. (2002) suggested that on inorganic membranes inorganic fouling may occur more easily. In general, a cake of inorganic matter can be irremovable due to the cohesive properties. More recently, Wang et al. (2008b) observed that the cake layer was formed by organic substances and inorganic elements such as Mg, Al, Fe, Ca, Si, etc. The organic foulants coupled with the inorganic precipitation enhance the formation of a cake layer. Lyko et al. (2007) also found that metal substance was a more signicant contributor to membrane fouling than biopolymers. Sometimes, the fouling caused by inorganic scaling is not easy to be eliminated even by chemical cleaning (You et al., 2006). These ndings indicate that inorganic fouling has become more and more important in MBRs. But, the understanding of inorganic fouling is still not clear. The investigation on the limiting concentration of metal ions in the feed wastewater that can lead to inorganic fouling will be of great interest, since the chemical composition of the wastewater is in close relation with the formation of precipitation. The inorganic fouling can form through two ways (see Fig. 6): chemical precipitation and biological precipitation. A great number of cations and anions such as Ca2, Mg2, Al3,

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2 3 Fe3, CO2 3 , SO4 , PO4 , OH and others are present in MBRs. Concentration polarisation will lead to higher concentration of retained salts on the membrane surface. Chemical precipitation occurs when the concentration of chemical species exceeds the saturation concentrations due to concentration polarisation. Additionally, the fouling layer on membranes can protect the surface layer from shear stress as biolm or biocake is elastic in nature leading to greater concentration polarisation and precipitation of inorganics (Sheikholaslami, 1999). Carbonates are one kind of the predominant salts in inorganic fouling. The aeration and the CO2 produced by microorganisms can affect the super-saturation of carbonates and the pH of the sludge suspension. The carbonates of metals such as Ca, Mg, and Fe can increase the potential of membrane scaling (You et al., 2005). Biological precipitation is another contribution to inorganic fouling. The biopolymers contain ionisable groups such 2 3 as COO, CO2 3 , SO4 , PO4 , OH . Metal ions can be easily captured by these negative ions. In some cases, calcium and acidic functional groups (RCOOH) can form complexes and build a dense bio-cake layer or gel layer that may exacerbate ux decline (Costa et al., 2006). When the metal ions in treated water pass through the membranes, they could be caught by the bio-cake layer via complexing and charge neutralisation and then accelerate membrane fouling. Metal ions play a signicant role in the formation of fouling layers, which can bridge the deposited cells and biopolymers and then form a dense cake layer. There exists a synergistic interaction among biofouling, organic fouling and inorganic fouling. Despite the fact that inorganic fouling is a troublesome phenomenon in MBRs, it is possible to avoid or limit inorganic fouling by pretreatment of feedwater and/or implementation of chemical cleaning. But the presence of a small quantity of metal ions such as calcium can be benecial for the membrane permeation in MBRs due to its positive effect on sludge occulation ability (Kim and Jang, 2006). As inorganic fouling can result in severe irremovable fouling, chemical cleaning is more effective than physical cleaning in the removal of inorganic precipitation. Chemical cleaning agents such as EDTA might efciently remove inorganics on the

membrane surface. EDTA can form a strong complex with Ca2, biopolymers associated with Ca2 ions are replaced by EDTA via a ligand exchange reaction (Al-Amoudi and Lovitt, 2007).

3.

Fouling factors and control strategies

The factors affecting membrane fouling can be classied into four groups (Le-Clech et al., 2006): membrane materials, biomass characteristics, feedwater characteristics, and operating conditions. The complex interactions between these aspects complicate the understanding of membrane fouling. For a given MBR process, the fouling behaviour is directly determined by sludge characteristics and hydrodynamic conditions. But, operating conditions (i.e., SRT, HRT and F/M) and feedwater have indirect actions on membrane fouling by modifying sludge characteristics. Table 3 gives the relationship between various fouling factors and membrane fouling on the basis of recent literature. In this review paper, the major fouling-causing factors including bound EPS, SMP, and hydrodynamic conditions are discussed. The fouling control strategies based on operating conditions and feedwater are proposed and summarized.

3.1. 3.1.1.

Bound EPS Denition of bound EPS and SMP

Chemical precipitation

Mn++nOH- M(OH)n Mn++CO32- MCO3 Mn++OH-+CO2 MCO3 Mn++SO42- MSO4 ------------

COOCOO
-

Biological precipitation

Mn+
COO-

EPS in either bound or soluble form are currently considered as the predominant cause of membrane fouling in MBRs. Bound EPS consist of proteins, polysaccharides, nucleic acids, lipids, humic acids, etc. which are located at or outside the cell surface. Soluble EPS and SMP are the same. SMP can be dened as the pool of organic compounds that are released into solution from substrate metabolism (usually with biomass growth) and biomass decay (Barker and Stuckey, 1999). Thus, SMP can be subdivided into two categories (Laspidou and Rittmann, 2002): substrate-utilisation-associated products (UAP), which are produced directly during substrate metabolism, and biomass-associated products (BAP), which are formed from biomass, presumably as part of decay. The interrelations between bound EPS and SMP are very complex. A unied theory for EPS and SMP was proposed by Laspidou and Rittmann (2002), who pointed out that cells use electrons from the electron-donor substrate to build active biomass, and they produce bound EPS and UAP in the process. Part of the bound EPS can be hydrolysed to BAP. Some SMP can be utilised by active biomass as recycled electron donors; and some can be adsorbed by the biomass ocs and then, become bound EPS. In addition, the generation of bound EPS and UAP is in proportion to substrate utilisation.

3.1.2.

Effect of bound EPS on membrane fouling

Sludge flocs

Colloids

Solutes

Crystal

Fig. 6 Schematic illustration of the formation of inorganic fouling in MBRs.

Bound EPS have been reported not only as major sludge oc components keeping the oc in a three-dimensional matrix, but also as key membrane foulants in MBR systems. Cho et al. (2005b) found a close relationship between the bound EPS and the specic cake resistance and established a functional equation in which the specic cake resistance was proportional to the EPS concentration. Ahmed et al. (2007) also

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Table 3 Relationship between various fouling factors and membrane fouling. Sludge condition
Sludge condition MLSS

Effect on membrane fouling

- MLSS[ / normalized permeabilityY - MLSS[ / fouling potential[ - MLSS[ / cake resistance[, specic cake resistanceY - Viscosity[ / membrane permeabilityY - MLSS/Viscosity[ / membrane permeabilityY - Viscosity[ / membrane resistance[ - F/M[ / fouling rates[ - MLSS (23 g/L): F/M[ / irremovable fouling[ MLSS (812 g/L): F/M[ / removable fouling[ - F/M[ / Protein in foulants[ - polysaccharide[ / fouling rate[ - bound EPS inuences on specic cake resistance - polysaccharide[ / fouling rate[ - bound EPS[ / membrane resistance[ - The loosely bound EPS contributes to most of the ltration resistance of the whole sludge - SMP is more important than MLSS - colloidal TOC relates with permeate ux - ltration resistance is determined by SMP - SMP is probably responsible for fouling - polysaccharide is a possible indicator of fouling - SMPY / fouling indexY - fouling rates correlate with SMP - lamentous bacteria[ / sludge viscosity[ - bulking sludge could cause a severe fouling - lamentous bacteriaY / cake resistanceY

Ref.
(Trussell et al., 2007) (Psoch and Schiewer, 2006a) (Chang and Kim, 2005) (Li et al., 2007a) (Trussell et al., 2007) (Chae et al., 2006) (Trussell et al., 2006) (Watanabe et al., 2006) (Kimura et al., 2005) (Drews et al., 2006) (Cho et al., 2005c) (Lesjean et al., 2005) (Chae et al., 2006) (Ramesh et al., 2007)

Viscosity

F/M

EPS

SMP

(Zhang et al., 2006b) (Fan et al., 2006) (Jeong et al., 2007) (Sperandio et al., 2005) (Le-Clech et al., 2005) (Jang et al., 2006) (Trussell et al., 2006) (Meng et al., 2007a) (Sun et al., 2007) (Kim and Jang, 2006)

Filamentous bacteria

Operating condition SRT

- SRT decrease from 100 to 20 d / TMP[ - SRT decrease from 30 to 10 d / fouling[ - SRTs[ / fouling potentials of SMP[ - SRT decrease from 5 to 3 d / fouling[ - HRTY / membrane fouling[ - HRTY / membrane fouling[ - HRTY / membrane fouling[ - aeration intensity[ / permeability[ - air-sparging improves membrane ux - larger bubbles for fouling control are preferable - air backwashing for fouling control is preferable - bubble-induced shear reduces fouling signicantly - air scouring can prolong membrane operation - sub-critical ux mitigates irremovable fouling - sub-critical ux mitigates fouling

(Ahmed et al., 2007) (Zhang et al., 2006b) (Liang et al., 2007) (Ng et al., 2006c) (Meng et al., 2007a) (Chae et al., 2006) (Cho et al., 2005a) (Trussell et al., 2007) (Psoch and Schiewer, 2006a) (Phattaranawik et al., 2007) (Chae et al., 2006) (Wicaksana et al., 2006) (Soa et al., 2004) (Lebegue et al., 2008) (Guo et al., 2007)

HRT

Aeration

Permeate ux

observed that as bound EPS concentration rose, the specic cake resistance increased, and this consequently resulted in the rise of TMP. A recent study by Ji and Zhou (2006) indicated that both composition and quantity of attached EPS on the membrane surface inuenced membrane fouling, and the total biopolymers in sludge suspension played a more important role than bound EPS in reecting the extent of membrane fouling. Ramesh et al. (2006) fractionated bound EPS into loosely bound EPS and tightly bound EPS, and proved that the fouling resistance was primarily caused by the loosely bound EPS, but not by the tightly bound EPS. The loosely bound EPS correlates with the performance of occulation and sedimentation processes (Li and Yang, 2007b).

Several studies, however, reported that bound EPS had little correlation with membrane fouling. Rosenberger and Kraume (2003) found that contrary to some literature, no impact of bound EPS on the lterability could be observed. Instead, the soluble EPS or SMP was found to have great impact on the lterability of sludge. This was conrmed by a more recent work reporting no clear relation between bound EPS and membrane fouling as its concentration was smaller than 10 mg/g SS (Yamato et al., 2006). In order to have a better understanding of sludge characteristics and their effects on membrane fouling, several investigations have been carried out (Germain et al., 2005; Fan et al., 2006). These investigations showed that activated sludge has very complex impacts on

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membrane fouling process. Bound EPS cannot be considered as the sole cause for membrane fouling, even though it has great effects on sludge characteristics and membrane fouling. Despite the fact that the research results on bound EPS are different from each other, it must be addressed that bound EPS concentrations are closely connected to sludge characteristics such as sludge volume index, occulation ability, hydrophobicity, surface charge, sludge viscosity. Therefore, considering the important roles of bound EPS in sludge characteristics and membrane fouling, bound EPS should be controlled in order to mitigate membrane fouling more efciently.

Fouling tendency
Ahmed et al. (2007) Lee et al. (2003) Zhang et al. (2006b) Han et al. (2005)

Ng et al. (2006b)

3 5

10

20

30

50

60

70

100

3.1.3.

Behaviour and control of bound EPS in MBRs

Optimum SRT
Fig. 7 Comparison of recent literature about the effects of SRT on fouling rate.

According to literature, there is no efcient approach to control the bound EPS directly since the MBRs include living microorganisms and their metabolites. Therefore, most of the recent reported literature is focused on nding suitable operating parameters in order to modify the sludge suspension. SRT is one of the most important operating parameters affecting MBR performance, in particular membrane fouling (Grelier et al., 2006). Cho et al. (2005b) reported that as SRT decreased, the amount of bound EPS in sludge ocs increased at MLSS condition of 5000 mg/L. A recent investigation reported by Ng et al. (2006b) showed that a longer SRT may improve membrane permeation (10-day and 20-day SRTs were better than 3-day and 5-day SRTs). They also observed that membrane fouling rate increased with rising SMP and bound EPS concentrations, both of which increased with decreasing SRT. Masse et al. (2006) found that bound EPS content decreased from 4570 to 2040 mg/gVSS when SRT increased from 10 to 53 d. The above-mentioned results suggest that too short SRT might do harm to membrane performance. A too long SRT, however, was also found to result in excessive membrane fouling. Lee et al. (2003) reported that as SRT increased from 20 days to 40 and 60 d, the overall fouling resistance increased. Han et al. (2005) also found that membrane fouling increased with increasing SRT (30, 50, 70, and 100 d) due to large amount of foulants and high sludge viscosity. Pollice et al. (2008) observed that the capillary suction time (CST) and sludge resistance to ltration (SRF) values, which are used to characterise the sludge lterability, were minimized for SRT in the range of 4080 d. These reported results indicate that in order to control bound EPS concentration and membrane fouling, the optimum SRT of MBRs should be controlled at 2050 d depending on HRT and feedwater (see Fig. 7). But some investigators observed that a long SRT will benet membrane permeation. Ahmed et al. (2007) reported that the membrane fouling became less when SRT increased from 20 days to 40, 60, and 100 d. The study was performed in an MBR equipped with a sequential anoxic/ anaerobic reactor for synthetic wastewater treatment. The contrary result probably results from this special MBR process. Sludge loading rate and correspondingly HRT and organic loading rate (OLR) are main operating parameters affecting the production of bound EPS since they govern biomass growth and decay. In addition, HRT can govern both the F/M of the bioreactor and the MLSS concentration. Meng et al. (2007a) reported that there were high bound EPS concentrations and high sludge viscosity as F/M ratio increased. The formation of

bound EPS is growth-related and is produced in direct proportion to substrate utilisation (Laspidou and Rittmann, 2002). Thus, the increase of organic loading rate or F/M ratio will induce the generation of more bound EPS. In addition, aeration intensity, dissolved oxygen and feed substrates have been proven as important parameters affecting bound EPS. With increased aeration rates, protein/carbohydrate ratios of sludge ocs decreased (Ji and Zhou, 2006). Li and Yang (2007b) used six lab-scale bioreactors to grow activated sludge with different carbon sources including glucose and sodium acetate, and different SRTs of 5, 10 and 20 d. The sludge that was fed on glucose had more EPS than the sludge that was fed on acetate. For any of the feeding substrates, the sludge had a nearly constant tightly bound EPS value regardless of the SRT, but the loosely bound EPS content decreased with the SRT, indicating that SRT is more important than feed substrates on the control of bound EPS. A more recent investigation also showed that the protein/carbohydrate (P/C 2, 4, and 8) ratios of feedwater correlated strongly with bound EPS composition (Arabi and Nakhla, 2008). It was found that with increasing P/C ratio of feedwater, the P/C ratio of bound EPS also increased slightly, but both protein and carbohydrate concentrations decreased. It can be concluded from these studies that there are several factors either alone or combined with each other that play an important role in the formation of bound EPS. It is of interest to know in what way the factor (SRT, HRT, F/M, DO, etc.) impacts on the formation of bound EPS. In recent years, lamentous bulking has been found to have a strong inuence on MBR fouling (Meng and Yang, 2007c; Su et al., 2007; Sun et al., 2007). The overgrowth of lamentous bacteria leads to a sharp increase of bound EPS concentration and then induces the increase of sludge viscosity and sludge hydrophobicity. In addition, the lamentous bacteria can enlace and x the foulants on the membrane surface (see Fig. 8). Sun et al. (2007) observed that with increasing sludge volume index (SVI), which results from lamentous bulking, the average increasing rate of TMP increased and the stable ltration period was shortened. Until now, there are only a few studies about the cause and control of lamentous bacteria in MBR processes, even though it

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exhibits signicant impacts on sludge characteristics and membrane fouling. Filamentous bulking can be controlled by selectors, optimisation of operating conditions, addition of coagulants and chlorine (Chudoba et al., 1973a,b; Caravelli et al., 2003). Another important approach for the control of lamentous bulking is to provide sufcient DO and alkalinity for the sludge, because in many cases the lamentous bulking is caused by the low DO of sludge suspension or low pH of feedwater (Liu and Liu, 2006). Another interesting approach for fouling control is the use of aerobic granular sludge membrane bioreactor (AGMBR) Because of the large size and dense structure, aerobic granular sludge has little chance to deposit on membranes, even though the granular sludge might have high bound EPS concentrations. Li et al. (2005b) reported that the membrane permeability of AGMBR was more than 50% higher than that of conventional MBR, but the AGMBR had more severe irremovable fouling, which resulted from the deposition of SMP (i.e., colloids and solutes) on membranes.

3.2. 3.2.1.

SMP Effect of SMP on membrane fouling

colloidal materials) was found to impact on fouling and to cause the difference in membrane performance between two identical MBRs. Iritani et al. (2007) reported that the relative contribution of the supernatant to the membrane fouling of an anaerobic activated sludge is nearly 100%, indicating that SMP is the controlling factor in microltration of activated sludge. But, the concentration of colloids and solutes in the supernatant was not mentioned in the paper. Lyko et al. (2007) analysed the SMP in supernatant and permeate as well as bound EPS extracted from fouled membranes in the full-scale MBR, and found an important inuence of soluble humic substances and carbohydrates in complexes with metal cations on membrane fouling. They also suggested that dissolved organic carbon (DOC) was an alternative to complex and costly measurements of SMP components (Lyko et al., 2008). These investigations suggest that the occurrence of SMP in MBRs impacts on membrane fouling signicantly, and SMP concentration and SMP composition would determine its fouling propensity. Furthermore, the occurrence of SMP in MBR efuent concerns the implementation of post-treatment for water recycling (e.g., the RO fouling in MBR RO process), and the discharge of SMPrich water brings additional troubles to local environment (e.g., the occurrence of dissolved organic nitrogen (DON)).

In fact, fouling behaviour cannot be attributed solely to bound EPS due to the complex nature of sludge suspension. Recently, the inuence of SMP on MBR fouling has attracted much attention (Rosenberger et al., 2005, 2006; Jeong et al., 2007; Drews et al., 2008; Paul and Hartung, 2008). Due to the membrane rejection, the SMP is more easily accumulated in MBRs, which results in the poor lterability of the sludge suspension. Geng and Hall (2007) observed that the oc size distribution and the amount of soluble EPS or SMP in the mixed liquor were the most important properties that significantly inuenced the fouling propensity of sludge, but the content of bound EPS was not found to be directly associated with membrane fouling. Furthermore, several attempts have shown that polysaccharide-like substances in SMP contribute to fouling more than protein-like substances (Rosenberger et al., 2006; Yigit et al., 2008). From Table 4 it also can be seen that the impacts of SMP on membrane fouling depend on SMP concentration, membrane materials and operation modes. Since SMP has been recognized as signicant membrane foulant, scientic research on SMP or sludge supernatant became one of the hot topics in membrane fouling. Rosenberger et al. (2006) reported that the SMP of the sludges (soluble and

3.2.2.

Behaviour and control of SMP in MBRs

SMP can accumulate on the membranes or penetrate into membrane pores. Accumulation and detachment of membrane foulants are determined by particle convection towards the membrane surface and the back transport rate of the deposited particles from membrane surface into the bulk. The back transport mechanisms in membrane ltration include inertial lift, shear-induced diffusion and Brownian diffusion. It is difcult to control the back transport of colloids and solutes only by enhancing aeration intensity due to the small size of these substances. The control of SMP concentration in MBRs is crucial. In general, the control of SMP can be achieved by two approaches: adjustment of operation parameters (i.e., SRT, HRT, DO concentration, temperature, aeration) and addition of adsorbents or coagulants to reduce SMP concentration.

3.2.2.1. Control of SMP via adjustment of operation conditions.

The effect of various process parameters on the production, accumulation and elimination of SMP is of considerable concern for researchers and engineers. Barker and Stuckey

Fig. 8 SEM images showing fouling cake layer formed with lamentous bulking sludge.

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(1999) summarized the process parameters (i.e., feed strength, HRT, OLR, SRT, substrate type, temperature, biomass concentration and reactor type) affecting the production of SMP in conventional activated sludge process. In MBRs, the cause and control of SMP formation were also investigated, especially in the recent few years. Shin and Kang (2003) reported that at an SRT of 20 d, an inuent DOC of 112 mg/L and an HRT of 6 h, the produced SMP was 4.7 mg DOC/L of which 57% was removed or retained by the membrane. At a long SRT, SMP concentration in the MBR reactor and efuent increased to some extent and then became stable, and nally decreased. Lee et al. (2003) found a decreasing contribution of the SMP to overall membrane fouling with increasing SRT (2060 d). Zhang et al. (2006b) operated a submerged MBR equipped with Kubota at-sheet membranes at a short SRT of 10 d and a moderate SRT of 30 d. During steady operation the total amount of EPS extracted from the ocs and the supernatant was approximately the same for the two SRTs under the same organic loading rate. However, the soluble polysaccharide concentration in the sludge suspension was about 100% higher for the SRT of 10 d than that for 30 d. More recently, Liang et al. (2007) presented an experimental study on SMP in MBR operation at different SRTs of 10, 20, and 40 d for the treatment of readily biodegradable synthetic wastewater. They observed that accumulation of SMP in the MBR became more pronounced at short SRTs. Similarly, Rosenberger et al. (2006) found that at an SRT of 8 d, the polysaccharide concentration varied in the range of 315 mg/L; while at an SRT of 15 d, it varied in the range of 38 mg/L. It can be seen that most of the reported results mentioned above showed that the SMP concentration decreased with increasing SRT. Therefore, it is feasible to control SMP concentration in MBRs by selecting suitable operation parameters. In MBRs, SMP are actually eliminated to a large extent via biodegradation, adsorption or other mechanisms (Drews et al., 2006). Drews et al. (2007) performed a comprehensive study to elucidate and quantify the effects of varying environmental conditions on SMP elimination. It was observed that DO and nitrate concentrations appeared to have an impact on SMP elimination and thereby on SMP concentration, with SMP elimination being lower at low DO concentration. At the same time, Min et al. (2007) observed that under DO limited conditions the sludge suspension contained a larger amount of high molecular weight compounds which lead to higher cake resistance. The low DO concentration could lead to poor occulation of individual activated sludge cells, so that the number of small particles in the sludge supernatant and soluble COD would increase as DO concentration decreased (Kang et al., 2003; Jin et al., 2006). As a result, a higher DO gave rise to a better lterability of sludge suspension (Kang et al., 2003). Sudden temperature changes led to spontaneous SMP release and increase in fouling rates (Drews et al., 2007). Morgan-Sagastume and Grant Allen (2005) found that deocculation of sludge ocs occurred under a temperature shift from 30 to 45  C, which caused an increase in turbidity and in SMP concentration. To achieve low SMP concentrations, a sufcient supply of oxygen is required in the bioreactor and sudden temperature change

The sludge samples from lab-scale MBRs were ltered in a batch test with a constant TMP of 27 kPa.

This study was performed in a cross-ow membrane ltration cell for 5 h with a constant TMP of 100 kPa.

This study was performed in a batch ltration unit for 4 h with a constant TMP of 4.0 kPa.

This study was tested in a cross-ow MBR. TMP 100 kPa, u 3 m/s, T 15  C, SRT 60 d MLSS 20.7 g/L, SRT 20 d (Wisniewski and Grasmick, 1998) (Defrance et al., 2000) (Bouhabila et al., 2001) 24 5 26

Remarks

SRT (Lee et al., 2003)

a These membranes were prepared with cellulose acetate (CA), N-methyl-2-pyrrolidone (NMP) and acetone. The compositions (CA/NMP/acetone) of CA-1, CA-2, CA-3, CA-4 are 15/35/50, 15/55/30, 15/75/10 and 15/85/0.

Table 4 Contributions of each sludge fraction to membrane fouling during membrane ltration of sludge suspension.

Solutes (%)

13 14 13 14 4 10 13 14

Colloids (%)

11 22 47

13 26 13

Flocs (%)

83 76 74 72

76 52 22

Bulking sludge Normal sludge Deocculated sludge Sludge characteristics (Meng and Yang, 2007c)

Membrane composition (Bae and Tak, 2005b)

20 days 40 days 60 days

CA-1 CA-2 CA-3 CA-4

63 72 71 52 65 24

37 28 29 24 30 50

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should be avoided (Drews et al., 2007). In addition, substrate type or feedwater composition affects the formation and elimination of SMP. McAdam et al. (2007) observed that carbon substrate had a great inuence on oc stability. Acetic acid resulted in the production of high concentrations of small particles (i.e., colloids and solutes) due to the weakly formed ocs. Ethanol, on the other hand, encouraged the growth of strong ocs that were capable of withstanding shear.

3.2.2.2. Control of SMP via addition of adsorbents/coagulants.

Addition of adsorbents or coagulants into sludge suspension can decrease the level of solutes and colloids or enhance the occulation ability. The addition of powered activated carbon (PAC) is a simple and convenient method for fouling control. The PAC can not only incorporate into the bioocs forming biologically activated carbon (BAC) (Ng et al., 2006a), but also adsorb biopolymers in the sludge suspension. The addition of PAC to MBRs provides a solid support for biomass growth, and hence reduces oc breakage (Hu and Stuckey, 2007). Moreover, the BAC ocs in MBRs are very strong and dense, which can help to prevent particle accumulation on the membranes. Akram and Stuckey (2008) studied the impacts of PAC addition on the performance of a submerged anaerobic MBR, and found that in the presence of 1.67 g-PAC/L, the combined effects of adsorption of ne colloids and solutes, and the formation of a thin cake layer resulted in signicant ux improvement from 2 to 9 L/(m2 h). However, the addition of 3.4 g-PAC/L reduced the ux to 5 L/(m2 h). As discussed by the authors, this evidence might be due to the increased sludge viscosity at high PAC addition. It suggests that PAC addition can improve membrane ux signicantly; but, if the addition of PAC is beyond the optimal value, it will do harm to membrane permeation. However, in some cases when the MBRs were operated without wastage the performance of the MBR(BAC) was worse than the conventional MBR. Thus, the improved performance of the MBR(BAC) requires regular replacement of aged BAC with fresh PAC (Ng et al., 2006a). Coagulants can remove SMP by charge neutralisation and bridging (Wu et al., 2006). Addition of an optimum calcium concentration could induce lower SMP concentration, lower hydrophobicity, lower concentration of lamentous bacteria and better occulation, which resulted in the reduction in cake layer resistance and pore blocking resistance (Kim and Jang, 2006). Attempts have been also made to use alum, ferric chloride, and chitosan as coagulants or lter aids (Iversen et al., 2008; Ji et al., 2008; Koseoglu et al., 2008; Song et al., 2008; Tian et al., 2008; Zhang et al., 2008c). Zhang et al. (2008c) reported that the addition of ferric chloride at the optimal concentration could reduce both SMP with MW > 10 kDa in the supernatant and the fraction of small particles (sludge ocs) in the range of 110 mm. The improvement of membrane ux or sludge lterability also depends on the coagulant used. Ji et al. (2008) found that the membrane fouling rate of the MBRs was in the order of Control MBR without coagulant > Al2(SO4)3 added MBR > Chitosan added MBR > Polymeric ferric sulfate (PFS) added MBR. In addition, cationic polymeric chemicals were found to be favorable due to their steady and successful performance in fouling control (Koseoglu et al., 2008). It has been reported that polymeric coagulants could supply more positive charges and longer

chain molecules, so that they had a better effect on lterability enhancement of sludge suspension than monomeric coagulants, while excess addition of polymeric coagulant led to colloidal re-stabilization (Wu et al., 2006). Recently, a so-called membrane fouling reducer (MFR) or membrane ux enhancer (MFE), which is a modied cationic polymer, has been developed to reduce membrane fouling in MBRs (Guo et al., 2008; Koseoglu et al., 2008). The addition of MFR can lead to the occulation of activated sludge. SMP is also entrapped by the microbial ocs during the course of the occulation, leading to an increase in the concentration of bound EPS (Hwang et al., 2007). With the addition of MFRs, the cost of aeration can decrease 4055% to achieve the same ux (Yoon et al., 2007). Lee et al. (2007) determined the optimum dosage as 0.025 mg/mg MLSS. But if the addition of MFR is beyond the optimum MFR dosage, soluble matters can be released from the microbial ocs to the bulk solution. Most MFRs and other additives have no or slight negative effect on the biomass activity (Iversen et al., 2008). These investigations further indicate that the addition of coagulants into sludge suspension is an effective and convenient method to control or eliminate SMP. But there are still many problems which need to be answered, such as the occurrence and fate of SMP in MBR, the change of SMP components after coagulants being added, the dynamic process of SMP production and elimination, and the accumulation and detachment of SMP on membranes. Moreover, the potential impacts of coagulants or adsorbents on biomass community or biomass metabolism need to be taken into account (Iversen et al., 2009), and the discharge of some chemicals that are used as coagulants or adsorbents might be a potential environmental risk. At this point, biomass-friendly coagulant or adsorbent (e.g., powdered activated carbon, chitosan) should be preferred unless the above-mentioned problems are made clear.

3.3.

Hydrodynamic conditions

3.3.1. Effect of hydrodynamic conditions on membrane fouling

Since submerged MBRs are more popular than cross-ow MBRs in scientic research and real applications, most of the recent studies on hydrodynamic conditions are focused on the reduction of aeration demand by enhancement of aeration efciency. In a cross-ow MBR, the membrane fouling can be limited by increasing cross-ow velocity. In a submerged MBR, shear stress is created by aeration, which not only provides oxygen to the biomass, but also maintains the solids in suspension and scours the membrane surface to alleviate membrane fouling. The aeration can be used to generate a shear stress on the membrane surface without requiring a recirculation pump. Hong et al. (2002) examined the effect of aeration on cake removal and suction pressure using a pilotscale submerged MBR and concluded that aeration was a signicant factor governing the ltration conditions. Previous investigation (Han et al., 2005) showed that the cakeremoving efciency of aeration did not increase proportionally with the increase in the airow rate and that the airow rate had an optimum value from the cake-removing point of view.

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Aeration is an important parameter determining both the size of the sludge ocs and the membrane ltration or fouling control. A high aeration rate certainly can reduce sludge attachment to the membranes, but it also has a signicant inuence on the biomass characteristics. Too high aeration intensity will lead to breakage of sludge ocs and production of SMP. Under high aeration intensity, the colloids and solutes would become the major membrane foulants (Fan and Zhou, 2007), because the resistance of colloids and solutes cannot be reduced effectively by increasing shear stress. The back transport of the colloids and solutes from the membrane surface is determined by Brownian diffusion, especially for solutes. The increase of aeration can improve shear-induced diffusion and inertial lift. Due to this the concentration gradients are steeper causing higher diffusion rates. The aeration intensity is expected to have a very complex inuence on MBR performance.

3.3.2. Favorable hydrodynamic conditions mitigating membrane fouling

In a low pressure membrane process, such as MBRs, the bubble size and bubble ow rate play signicant roles in hydrodynamic conditions and energy demand. Fane et al. (2005) compared the effect of two nozzle sizes, 0.5 and 1.0 mm diameter, on bubble size and membrane fouling. The larger nozzle could produce higher bubble sizes than the smaller nozzle. However, the fouling control, characterised by dTMP/dt, was noticeably improved using the smaller nozzle with the smaller bubbles. A more recent study by Prieske et al. (2008), however, suggests that the smaller bubble size (1 mm) could induce a slower circulation velocity than large bubbles (2 and 3 mm) due to a higher gas holdup in the downcomer, and concluded that larger bubbles seem to be more efcient for air scour of the membrane surface because the resulting drag and lift forces on the membranes are much higher due to higher circulation velocities. It also has been reported that fouling reduction increased with the airow rates up to a given value and beyond this ow rate no further enhancement was achieved (Ndinisa et al., 2006a). In addition, under certain conditions intermittent airow can achieve better fouling control than continuous ltration and it also reduces energy requirements. For submerged hollow bers in bubble-enhanced systems, such as the membrane bioreactor, the preferred ber orientation should be vertical rather than horizontal though the overall effect of ber orientation on ltration is smaller than the turbulence caused by the two-phase ow (Chang et al., 2002b). The size of the gap between the submerged at-sheet membranes is also important for two-phase ow and fouling control (Ndinisa et al., 2006a). As the gap was increased from 7 mm to 14 mm, the fouling became worse and the degree of fouling reduction by two-phase ow decreased by at least 40% based on suction pressure rise (dTMP/dt). Moreover, ber movement and fouling control are inuenced by ber tightness with signicantly improved performance for slightly loose bers (Wicaksana et al., 2006). In recent years, to look for a more efcient membrane fouling control, air-sparging in MBRs has been paid more and more attention to (Delgado et al., 2008; Psoch and Schiewer, 2008). The benets of air-

sparging are the enhancement of hydrodynamic conditions and the efcient use of aeration. The interaction of two-phase ow with membranes in MBRs is a complex issue. During the last few years, the analysis of the hydrodynamics and the uid ow pattern adjacent to the membrane have been studied and visualised by CFD mathematical modeling and simulation (e.g., Ahmad et al., 2005). The multi-phase ow simulation by CFD technique can provide microscopic understanding of the fouling mechanism, and it has been proven to be a powerful tool to aid membrane module design (Li et al., 2006). Ndinisa et al. (2006b) studied the fouling in a submerged at sheet MBR using twophase ow characterisation and CFD simulation. It was found that the ux enhancement by the increasing bubble size was primarily due to an increase in the overall shear stress on the membrane and to more turbulence generated by introduction of the gas phase. In addition to aeration intensity, the rheological properties of sludge suspension not only have major impacts on oxygen transfer and sludge conditioning in the next step, but also have a strong inuence on transport phenomena near the membrane surface. For a given aeration intensity, the increase of sludge viscosity will weaken the hydrodynamic conditions close to the membranes. An example is the sharp decrease of the shear stress at the membrane surface with increasing sludge viscosity (Meng et al., 2007b). According to the rheological properties of activated sludge, Van Kaam et al. (2008) proposed an intermittent aeration mode, which allows activated sludge to restructure and can effectively prevent MBR fouling. Of particular interest is the energy saving of the intermittent aeration. In brief, enhancement of hydrodynamic conditions is one of the effective approaches to mitigate membrane fouling in MBRs. But, the hydrodynamic conditions has close relation with aeration intensity, bubble size, membrane module conguration, MLSS concentration and sludge viscosity, etc. Therefore, the hydrodynamic conditions in MBRs is very complex; and optimisation of membrane module and aeration combined with CFD modeling and simulation might be helpful for the improvement of the hydrodynamic conditions. Besides bound EPS, SMP and hydrodynamic conditions we mentioned above, attempts have been made to control fouling or modify sludge by using ultrasound, ozone and electric eld (Chen et al., 2007; Huang and Wu, 2008; Sui et al., 2008; Wen et al., 2008). Experimental results showed that ultrasound could control membrane fouling effectively although membrane damage may occur under some operation conditions (Wen et al., 2008). One interesting method is the use of an electric eld, which could prevent the sludge ocs and colloids depositing onto the membrane surface. In addition, attempts also have been made to control MBR fouling by developing novel ltration modes and/or backwashing conditions (Wu et al., 2008a,b).

3.4.

Summary

So far, there is a great number of investigations focused on membrane fouling, most of which still consider bound EPS, SMP and hydrodynamic conditions as the main factors affecting membrane fouling. At least, these investigations

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indicate that membrane fouling has more or less relation with the above-mentioned factors. The adjustment of operating conditions or feedwater can be used to modify sludge characteristics (e.g., SMP) and then control membrane fouling. Table 5 presents the fouling control strategies based on various fouling factors. A schematic illustration about favorable conditions mitigating membrane fouling is also given in Fig. 9. Regarding the discussion about other fouling factors such as MLSS concentration, sludge viscosity and sludge particle size, it can be found in recent review papers (Chang et al., 2002a; Le-Clech et al., 2006).

Table 5 Summarization of fouling control strategies based on various fouling factors. Control strategy
Hydraulic control

Control item and its effect on membrane fouling factor

- HRTY / sludge viscosity[ (Meng et al., 2007a), EPS[ (Chae et al., 2006) - aeration[ / permeability[ (Psoch and Schiewer, 2006a; Trussell et al., 2007), ber movement[ (Wicaksana et al., 2006), cake-removing efciency[ (Chang and Judd, 2003), and cake resistanceY (Psoch and Schiewer, 2006b; Fan and Zhou, 2007) - periodical backwashing / ux[ (Psoch and Schiewer, 2006a) and operation period[ (Chae et al., 2006), total resistanceY (Psoch and Schiewer, 2006b) - sub-critical/low ux operation / sustainable operation (Bacchin et al., 2006; Guglielmi et al., 2007a) - powdered activated carbon / EPSY (Ying and Ping, 2006), irremovable foulingY (Ng et al., 2006a; Ying and Ping, 2006) - membrane fouling reducer / cake porosity[, soluble EPSY (Hwang et al., 2007; Lee et al., 2007) - occulation/coagulation / organic matterY (Zhang et al., 2008c) - chemically enhanced backwashing / remove fouling (Kim et al., 2007) - SRT[ / bound EPSY (Ahmed et al., 2007), SMPY (Liang et al., 2007) - MLSS/viscosityY / permeate ux[ (Li et al., 2007a; Trussell et al., 2007), cake foulingY (Chang and Kim, 2005; Chae et al., 2006) - F/M ratioY / fouling resistanceY (Trussell et al., 2006) - lamentous bacteriaY / bound EPSY (Meng et al., 2006a)

4.

Developments of membranes/lters

4.1. Inuence of membrane characteristics on MBR performance

Membrane characteristics such as pore size, porosity, surface charge, roughness, and hydrophilicity/hydrophobicity, etc., have been proven to impact on MBR performance, especially on membrane fouling. The determination of suitable membrane pore sizes has been extensively investigated in the 1990s. Pore size distribution is likely to be one of the parameters affecting membrane performance. A narrow pore size distribution is preferred to control membrane fouling both in MBR process and in conventional membrane separation process. The membrane materials always show different fouling propensity due to their different pore size, morphology and hydrophobicity. Polyvinylidene uoride (PVDF) membrane is superior to polyethylene (PE) membrane in terms of prevention of irremovable fouling in MBRs used for the treatment of municipal wastewater (Yamato et al., 2006). Regarding MBR processes, the fouling behaviour of the membrane used is determined by the afnity between foulants (e.g., EPS/SMP) and membrane. Zhang et al. (2008b) studied the afnity between EPS and three polymeric ultraltration membranes, and observed that the afnity capability of the three membrane was of the order: Polyacrylonitrile (PAN) < PVDF < Polyethersulfone (PES). It suggests that among these membranes the PAN membrane is more fouling-resistant. Inorganic membranes, such as aluminum, zirconium, and titanium oxide, show superior hydraulic, thermal, and chemical resistance. A stainless steel membrane was used for MBR, and the result showed that the stainless steel membrane could obtain a higher permeate ux (Zhang et al., 2005b), and it is a potential alternative for the treatment of high temperature wastewater (Zhang et al., 2006d). In the stainless steel membrane bioreactor, thermophilic bacteria could be cultivated when the MBR was operated at higher temperature. But, these inorganic membranes are not the preferred option for large-scale MBR plants because of their high costs. In addition, inorganic membranes can induce severe inorganic fouling (i.e., struvite formation). So, the inorganic membranes might be used only in some special applications such as high temperature wastewater treatment. In general, membrane fouling occurs more readily on hydrophobic membranes than on hydrophilic ones because of the hydrophobic interaction between foulants and membranes As a result, much attention has been given to reduce membrane
Chemical control

Biological control

fouling by modifying hydrophobic membranes to relatively hydrophilic (Yu et al., 2005a,b). The objective of this paper is to review the recent and current developments of membranes in MBRs, so the main content of Section 4 is focused on the novel and signicant ndings in membranes or lters used for MBRs. The detailed discussion on the impacts of membrane material

Fig. 9 Favorable conditions mitigating membrane fouling.

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on membrane fouling can be found in recent reviews (Chang et al., 2002a; Le-Clech et al., 2006).

4.2.

Application of low-cost lters

Both capital and operation costs of the MBRs must be reduced in order to increase their competitiveness with respect to conventional activated sludge processes. In MBRs, the membranes are just used as lters, which have small pores. Since an improved efuent quality might not always be required and only standard criteria are stipulated, it should be feasible to substitute the membranes by cheaper lters with large pore size. The low-cost lters investigated include (Ye et al., 2006; Iversen et al., 2007; Seo et al., 2007; Satyawali and Balakrishnan, 2008): non-wovens, meshes and lter cloths. Non-wovens are composed of a random network of overlapping bers having multiple connected pores through which the uid can ow (Chang et al., 2006). Due to its large pore size or porosity, the non-woven could obtain a high-ux even at very low pressure. There are little differences in the efuent water quality between the non-woven bioreactor and the membrane bioreactor (Meng et al., 2005). In 1998, non-woven and coarse pore lter modules were applied in the pilot-scale and full-scale wastewater treatment plant in Tokyo (Asou et al., 1998). The performance of both pilot-scale and full-scale plants was acceptable for real municipal wastewater. Then, Seo et al. (2003) in Korea developed an anaerobic/aerobic bioreactor in which a non-woven module was submerged into the aerobic compartment. The COD removal efciency was 91.6% producing an efuent COD concentration around 13 mg/L. These results conrmed that non-wovens can be used in wastewater treatment processes to substitute the membranes, though it cannot be compared with conventional membranes in some cases. But, as a new lter used in wastewater treatment process, the non-woven still has its own shortcomings. Compared with polymeric membranes, some non-woven lters have a lower tensile strength and tear strength, and a lower resistance to microbiological corrosion. It is, therefore, expected that the lifetime of non-woven lters, which depends on the material, might be small. Mesh bioreactors are potential processes used for wastewater treatment, especially when a small area requirement is a high priority (Kiso et al., 2005). Fuchs et al. (2005) obtained a much higher ux of 50150 L/(m2 h) at very low pressure depending on operating conditions (i.e., MLSS concentration, aeration, HRT). Due to the much larger pore size of the mesh, the efuent of a mesh bioreactor is not of the same excellent quality as that of a membrane bioreactor (Fuchs et al., 2005; Wang et al., 2006). But, a self-forming dynamic membrane (SFDM) forms on the coarse mesh during the ltration of activated sludge (Fan and Huang, 2002). As soon as the SFDM is formed, it can improve efuent quality signicantly. Besides the low cost, it can be concluded that the high permeation at very low suction pressure is another attractive character of these lters. The major problem limiting the application of low-cost lters is the severe fouling due to their rough surface and the too large pore size. The sludge ocs can entrap in the void among the ber matrix and it is difcult to be removed by shear stress. Due to the large pore size, pore blocking by

sludge ocs is one of the main reasons leading to lter fouling (Moghaddam et al., 2006). In order to avoid the rapid decline of permeate ux of lter cloth, Ye et al. (2006) precoated the lter cloth with powdered activated carbon (PAC) before submerging it into a bioreactor. It was found that the precoated lter could not only mitigate membrane fouling, but improve the efuent quality signicantly as well. It indicates that the severe fouling of low-cost lters can be resolved by modifying the lters to improve the surface roughness, hydrophilicity, surface charge and so on (see Section 4.3).

4.3.

Membrane modication

The main objective of new membrane material development is to reduce the high cost of investment for the membrane modules or to enhance and maintain membrane ux. To improve the anti-fouling property of polypropylene hollow ber microporous membranes (PPHFMMs) in an MBR for wastewater treatment, the PPHFMMs were subjected to surface modication by NH3 and CO2 plasma treatment by Yu et al. (2005a,b, 2008). The water contact angle reduced signicantly after NH3 and CO2 plasma treatment because NH2 groups and COOH groups were grafted on the membrane surface. Fouling indices of the NH3 and CO2 plasma treated PPHFMMs were lower than those of the unmodied PPHFMMs. Although the plasma treatment processes have many advantages, such as a very shallow modication depth compared to other surface modication techniques, it still has drawbacks. For example, the chemical reactions of the plasma treatment are rather complex, so the surface chemistry of the modied surface is difcult to understand in detail and thus, currently it is not possible to extend plasma treatment on large-scale (Yu et al., 2007). To overcome these disadvantages of plasma treatment, Yu et al. (2007) applied the surface graft polymerisation method to improve the membrane permeation in MBRs. In the study, the surface modication of polypropylene microporous membranes was accomplished by UV irradiation in aqueous acrylamide solutions. The contact angle data showed that the hydrophilicity of the surface modied membranes increased strongly with the increase of the grafting degree. Even though the modied membrane showed better ltration ability in the MBR than the unmodied membrane, this method has the disadvantage of employing high-energy methods, such as UV irradiation, plasma treatment, gamma irradiation, and chemical reaction, resulting in an increase in membrane production cost (Asatekin et al., 2006). Recently, a self-assembly technique, which is one of the simplest and most effective methods to prepare a thin lm on the membrane surface, was employed for fabricating a fouling resistance membrane in MBR (Asatekin et al., 2006). In this study, commercial polyvinylidene uoride ultraltration membranes (PVDF UF) were coated with the amphiphilic graft copolymer polyvinylidene uoride-graft-polyoxyethylene methacrylated (PVDF-g-POEM), to create thin lm composite nanoltration membranes (TFC NF). The new TFC NF membranes exhibited no irremovable fouling in 10-day deadend ltration of model EPS (bovine serum albumin, sodium alginate and humic acid) at concentrations of 1000 mg/L. The anti-fouling properties of the TFC NF membranes were

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attributed to both the nanoscale dimensions of the hydrophilic channels through the coating, which greatly restrict the size of permeate species, and the unique properties of polyethylene oxide (PEO), which can resist the adsorption of EPS on the membrane surface. Meanwhile, TiO2 embedded polymeric membranes have been prepared by a self-assembly process and applied to the ltration of MBR sludge (Bae and Tak, 2005a,c). The surface of a TiO2 embedded membrane can was more hydrophilic than that of neat polymeric membrane due to the higher afnity of metal oxides to water. Therefore, hydrophobic adsorption between sludge suspension and TiO2 embedded membrane can be reduced, and deposited foulants are readily removed by cross-ow (Bae and Tak, 2005a,c). They conrmed that self-assembly technique can be successfully used to modify the membranes for membrane fouling control in MBRs. Recently, Zhang et al. (2008a) attempted to modify non-woven lter by dip-coating PVA (polyvinyl alcohol). The results obtained from two parallel MBRs indicated that the ux decline of modied non-woven lter was only 12%, in comparison of the original non-woven lter of 40%. In addition to membrane modication, the development of economical, high-ux, non-fouling membranes is still needed before viable MBR processes can be achieved (Shannon et al., 2008). The non-fouling or low-fouling membrane should have much narrower pore size distributions, stronger hydrophilicity, and larger porosity than the currently used membranes. At this point, the microsieve membrane, which has very uniform pore size (Brans et al., 2006; Ning Koh et al., 2008), can provide a useful alternative for the development of narrow pore size distribution membranes. On the other hand, nanotechnology might be of interest for the development of strong hydrophilic membranes.

4.4.

Dynamic membranes

In recent years, dynamic membranes have been investigated in MBRs in order to improve membrane performance. Dynamic membranes were rstly reported in 1965 by investigators at the Oak Ridge Laboratories engaged in desalination research (Marcinko et al., 1966). Dynamic membranes can be prepared by ltering a solution containing either inorganic or organic materials through a porous support (Fan and Huang, 2002). There are two basic types of dynamic membranes: precoated and self-forming. The precoated membrane is produced by passing a solution of one or more specic components over the surface of a porous support. The selfforming membrane is formed by the components in the solution to be ltered. Many hydrated oxides, natural polyelectrolytes, and synthetic organic polymers can be used for the preparation of precoated membranes. It has been also reported that modied membranes coated with an even PVA hydrogel layer show dramatically high anti-fouling characteristics and good ux recovery compared to inadequately modied membranes and unmodied membranes (Na et al., 2000). Although these investigations were based on conventional membrane separation, they provide valuable information for the application of dynamic membrane in MBRs. The precoated dynamic membrane bioreactor was rstly reported by Li et al. (2005a), who prepared the dynamic

membrane by circulating kaolinite suspension through the ceramic membrane module to improve MBR performance. The precoated dynamic membrane bioreactor had satisfying performance on organic substances and nitrogen removal. But, the inuence of precoated membranes on fouling or rejection was not discussed. Ye et al. (2006) proposed a precoated dynamic membrane bioreactor used for municipal wastewater treatment. The lter cloth with a pore size of 56 mm and powdered activated carbon were used as support lter and precoating reagent. It was found that during the long-term operation the removal efciencies of organic carbon and ammonia were as good as traditional hollow ber membrane bioreactors. The precoated lter cloth had a more excellent performance with respect to fouling control than uncoated lter cloth and hollow ber membranes (Zhang et al., 2005a). In addition, the precoated membrane had a low irremovable fouling during the operation of MBRs. This nding coincides with a previous study (de Amorim and Ramos, 2006). It suggests that precoated dynamic membranes can help to improve the lterability of lter cloths, mesh lters and nonwoven lters, so it provides these low-cost lters with a larger potential in MBRs. Self-forming dynamic membranes were rstly used in conventional membrane separation process. The self-forming dynamic membrane implies that the rate of particle convection towards the membrane surface is balanced by the rate of back transport. The self-forming dynamic membrane can improve both the permeate ux and rejection of solutions. The performance of self-forming dynamic membranes is determined by concentration, type, shape, molecular weight of ltering solution and cross-ow velocity. Currently, self-forming dynamic membranes have been introduced into MBRs in order to explain the formation and action of bio-cake layer on the membrane surface. A study by Lee et al. (2001) gave an explanation about self-forming dynamic membranes in MBRs. As the membrane ltration reaches a steady state, a dynamic membrane will have been formed, which mainly consists of large sludge ocs. It was reported that the fouling layers forming on the membrane surface act as barriers which protect membrane surfaces and pores from being fouled (Lee et al., 2001) because EPS, soluble organics and colloidal particles could be rejected or biodegraded by the dynamic membrane composed of living microorganisms. Thus, the foulants have fewer chances to deposit on the membrane surface. Fan and Huang (2002) reported self-forming dynamic membranes formed on a 100 mm coarse mesh instead of MF or UF membranes. The gel layer formed on the mesh surface had a structure like conventional membranes and played a key role in the selfforming dynamic membrane. From these reported ndings, it can be expected that that self-forming dynamic membranes can not only mitigate membrane fouling in MBR, but also provide an alternative to improve the performance of some cheaper lters (i.e., lter cloth, non-woven, coarse mesh). It should be pointed out that the performance of the dynamic membrane is dependent upon many factors such as cake density, cake structure and cake components. For example, when the cake layer formed on the membrane surface becomes thick, the oxygen in the bulk cannot be transported into the inner regions of the cake (Zhou et al., 2008) and then

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the bacteria will lose their activity and release a great deal of biopolymers. In such case, the so-called dynamic membrane will lead to severe membrane fouling.

5.

Conclusions and perspectives

In this paper, recent advances of research on membrane fouling and membrane material in MBRs were reviewed. From the viewpoint of fouling reversibility with physical and chemical cleanings, membrane fouling includes removable and irremovable fouling, in which the latter will be paid more and more attention to in MBRs, especially in long-term operation. From the viewpoint of fouling components, the fouling in MBRs can be classied into three major categories: biofouling, organic fouling and inorganic fouling. The results obtained from recent investigations on bound EPS, SMP, lamentous bacteria and hydrodynamic conditions are updated. In the coming few years, membrane fouling is still a hot issue in research and application of MBRs. According to recent literature and our own experience, the future study on membrane fouling should include: (1) Studies on membrane fouling mechanisms should focus on identication and characterisation of membrane foulants (i.e., chemical and biological components of foulants, bacteria community of the foulants). Cake formation, pore blocking, and EPS/SMP adsorption on/within the membranes could all be important. Of particular importance could be the interaction and interrelation between these mechanisms and sludge characteristics. (2) Development of procedures for the visualisation and characterisation of membrane fouling in MBRs. Direct monitoring and in situ techniques will offer more useful information about the formation of membrane foulants. (3) Development of more effective and easy methods to control and minimize membrane fouling. Generally, removable fouling is controlled by creating shear stress on the membrane surface. Although air bubbles are used to promote shear stress and to enhance the membrane ux, they also have strong impact on biomass characteristics. Moreover, enforced aeration will need more energy. Research should be directed to optimisation of the current coarse aeration methods for submerged membrane modules. Lastly, alternative ltration concepts to limit the deposition of foulants onto the membrane surface should be developed. (4) Study the fouling behaviour in full-scale MBR plants in order to reect the real fouling behaviour. (5) Development of novel membrane modules for MBRs to reduce their capital costs and enhance their hydrodynamic conditions. (6) Modeling of mass transfer and membrane fouling by mathematical approaches such as CFD, Monte Carlo simulation, fractal theory, articial neural network (ANN). In other words, a comprehensive investigation should be performed to understand, control and reduce membrane fouling, especially avoiding severe fouling; it is just like a systematic physical examination on a person to understand

his/her health condition and to avoid the occurrence of illness, especially fatal diseases. In recent years, there are considerable investigations about the impacts of membrane materials, pore size, hydrophilicity/ hydrophobicity, etc., on membrane fouling; however, most of the recent investigations are focused on the application of low-cost lters to substitute the membranes, modication of membranes to enhance their hydrophilicity and use of dynamic membranes to improve the performance of membranes or low-cost lters. In the future, to our knowledge, the study on membrane materials in MBRs should still focus on: (1) Development of anti-fouling membranes or modication of current membranes. (2) Enhancement of the performance of low-cost lters by modifying their surface properties.

Acknowledgements
The rst author is a research fellow of the Alexander von Humboldt Foundation. This work is partially supported by Alexander von Humboldt Foundation (07.200712.2008).

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