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
a

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 Universitat 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

article info

abstract

Article history:

Membrane bioreactors (MBRs) have been actively employed for municipal and industrial

Received 7 April 2008

wastewater treatments. So far, membrane fouling and the high cost of membranes are

Received in revised form

main obstacles for wider application of MBRs. Over the past few years, considerable

19 December 2008

investigations have been performed to understand MBR fouling in detail and to develop

Accepted 22 December 2008

high-flux or low-cost membranes. This review attempted to address the recent and current

Published online 3 January 2009

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

Keywords:

control strategies were discussed. Recent developments in membrane materials including

Membrane bioreactor (MBR)

low-cost filters, membrane modification and dynamic membranes were also reviewed.

Membrane fouling

Lastly, the future trends in membrane fouling research and membrane material develop-

Extracellular polymeric substances

ment in the coming years were addressed.

(EPS)

2009 Elsevier Ltd. All rights reserved.

Soluble microbial products (SMP)

Membrane modification

Abbreviations: AFM, atomic force microscopy; AGMBR, aerobic granular sludge membrane bioreactor; ANN, artificial neural network;
BAC, biologically activated carbon; BAP, biomass-associated products; BOD, biological oxygen demand; CFD, computational fluid
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, fluorescence in situ
hybridization; FTIR, Fourier transform infrared spectroscopy; HP-SEC, high performance size exclusion chromatography; HRT, hydraulic
retention time; MBR, membrane bioreactor; MF, microfiltration; MFE, membrane flux enhancer; MFR, membrane fouling reducer; MLSS,
mixed liquid suspended solid; NF, nanofiltration; 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 fiber microporous membrane; PVDF, polyvinylidene fluoride;
RO, reverse osmosis; SEM, scanning electron microscopy; SMP, soluble microbial products; SRF, sludge resistance to filtration; SRT, solid
retention time; TFC, thin film composite; TMP, transmembrane pressure; UAP, substrate-utilisation-associated products; UF, ultrafiltration; 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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water research 43 (2009) 14891512

Contents

3.

4.

5.

1.

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 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

Introduction

MBRs are being increasingly used for wastewater treatment

that requires excellent effluent 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 efficiency 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 significant 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

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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

1.
2.

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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water research 43 (2009) 14891512

Biomass-related aspects

MBR fouling
(Foulants)

Activated
sludge
Determine
fouling

Control
fouling

Modify
sludge

Aeration,
Cleaning

SRT, HRT, F/M,

DO, OLR
Operation conditions

Fig. 2 Schematic illustration showing the fouling affecting

factors and controlling approaches.

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 find out the effective approaches (e.g., suitable
operating parameters) for the modification of activated
sludge, the influence 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
findings such as the influence of filamentous bulking on MBR
fouling and the use of computational fluid dynamics (CFD).
Lastly, the development of new membrane/filter 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

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 flux 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 flocs 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
defined 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 flux due to fouling
eventually causing local fluxes to be higher than the critical
flux. Latterly, Zhang et al. (2006a) reported that the sudden
jump was possibly not only due to the local flux effect, but also
caused by sudden changes of the biofilm or cake layer structure. Due to oxygen transfer limitation, the bacteria in the
inner biofilms tend to die and release more extracellular
polymeric substances (EPS). A more recent investigation also
confirmed 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 fluxes
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

b
Sludge particles
Colloids
Solutes

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

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water research 43 (2009) 14891512

TMP

TMP Jump

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

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
flux (e.g., operation below critical flux).
In MBRs, the prediction or measurement of fouling resistance is significant for the understanding of fouling extent, or
for the optimisation of operating conditions. Furthermore, the
knowledge of the filtration mechanisms can help to find 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 flux or membrane fouling resistance in
MBRs. These empirical models are helpful for the understanding and mitigation of membrane fouling 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.

Membrane fouling is a very complicated phenomenon and
results from multiple causes. Particle sizes of sludge flocs,
colloids and solutes in mixed liquor may strongly affect
fouling mechanisms in a membrane filtration 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 flocs 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 definitions
proposed in publications. Generally, the irreversible fouling
should be defined as the fouling that cannot be removed by
any methods including chemical cleaning. But, some previous
studies defined the irreversible fouling as the fouling that can
be removed by chemical cleaning but cannot be removed by
physical cleaning. Here, we define three types of fouling:

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
filtration. 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.

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 filtration 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 scientific 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 fibers. 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 film that was frequently washed
away by aeration turbulence. The filtration resistances of the
sludge cake and thin sludge film 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 flocs more tightly on
the membrane and increases the difficulty 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 flux close to the critical flux. The consolidated cake could not be removed by the back-flush 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 flow field by using the
three-dimensional volumetric grid model and confocal laser
scanning microscopy (CLSM) analysis, and observed that there
was a very complex flow pattern in the fouling layer. Because
of the inter-connectivity of the neighboring pores, the flow
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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water research 43 (2009) 14891512

Table 1 Expressions developed to describe membrane flux or membrane fouling resistance (modified after Judd and
Jefferson, 2003).
Application

Expressiona

DP
Classical cake J
mRm aCMLSS
filtration

Remarks
2

J is membrane flux (L/m h), DP is TMP, CMLSS is the

biomass concentration (mg/L), m is sludge viscosity
(mPa s), a is specific 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-flow
J 
CMLSS is sludge concentration (mg/L), CCOD is COD value
1:37 0:326
m Rm 843DPC0:926
MBR
(mg/L), m is sludge viscosity (mPa s).
MLSS CCOD m


MLSS is sludge concentration (kg/m3), MLVSS is volatile
Cross-flow
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
flux (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 specific 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
efficiency of cross-flow velocity, ranging from 0 to 1.
0:532
Submerged
K 8:93  107  CMLSS
 J0:376  Ua3:05
K is the increasing rate of filtration resistance (1/(m h)), X is
MBR
sludge concentration (mg/L), J is membrane flux (L/m2 h),
ULr is observed cross-flow 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 filtration 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).

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
filtration, 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 significance for MBR operation.
Operation below the critical flux is an effective approach to
avoid severe fouling including removal and irremovable
fouling within a given filtration system. Field et al. (1995)
introduced critical flux concept, operation below the critical
flux concept is called sub-critical flux or non-fouling operation
and is expected to lead to little irremovable fouling. For
a short-term membrane filtration, when the permeate flux is
set below the critical flux, the TMP remains stable and fouling
was removable. In contrast, when it exceeds the critical flux,
the TMP increases and might lead to a TMP jump. As a matter
of fact, for a long-term operation of MBRs, irremovable fouling

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)

(Nagaoka et al., 1998)

(Lee et al., 2002)

(Liu et al., 2003)

(Meng et al., 2006b)

can occur even if they are operated below the critical flux.
Ognier et al. (2004) reported that despite the initial choice of
sub-critical flux filtration conditions, gradual fouling was seen
to develop which, after long periods of operation without
intermediary membrane regeneration, proved to be hydraulically irremovable. The critical flux value depends on
membrane characteristics, operating conditions (i.e., aeration
intensity, temperature), and sludge characteristics. Further
discussion of critical flux can be found in recent review articles (Pollice et al., 2005; Bacchin et al., 2006). The concept of
critical flux 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 flux 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 flux 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 flux or
removable/irremovable fouling. It is also of high interest to
develop a unified 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

1494

water research 43 (2009) 14891512

New membrane

Irreversible fouling

Initial filtration
Chemical cleaning

Long-term filtration

Physical cleaning

Removable fouling
irremovable fouling

and

Sludge flocs

Irremovable fouling
Colloids

Solutes

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 classified 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

Effect of cake layer

on membrane fouling

Ref.

Synthetic
wastewater

- Cake formation was entirely

governing the applicable flux

(Jeison and
van Lier,
2007)

Municipal
wastewater

- The resistance of cake layer

accounts for 9598% of the total
filtration resistances
(sludge filtration)
- The specific filtration 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

(Ramesh
et al., 2007)

- At high permeate flux, cake

resistance (Rc) prevailed internal
fouling resistance (Rf). At low
permeate flux, Rf affect more
greatly than Rc

(Shin et al.,
2005)

Agricultural
wastewater

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

(Chu and Li,

2006)

foulants will help us to propose more effective approaches for

fouling control. Biofouling refers to the deposition, growth and
metabolism of bacteria cells or flocs on the membranes, which
has aroused a significant concern in membrane filtration
processes (Pang et al., 2005; Wang et al., 2005). For a low
pressure membrane such as microfiltration and ultrafiltration
for treating wastewater, biofouling is a major problem
because most foulants (microbial flocs) 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 flocs (Li et al., 2003; Zhang et al.,
2006a). Zhang et al. (2006a) used a DOTM to observe the
interactions between the bioflocs and the membrane surface.
The images showed that the bioflocs 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 biofilm structure and analysed its effect on membrane permeability in MBR for dye
wastewater treatment. They found that membrane filterability was closely associated with the structural parameters
of the biofilms (i.e., porosity, biovolume). The visualisation of
biofouling using these techniques is helpful for understanding
of the floc/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

water research 43 (2009) 14891512

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 specific
phylogenetic group of bacteria, the Betaproteobacteria, probably
played a major role in development of the mature biofilms,
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 affinity 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 bioflocs/cells and mechanisms of
cell attachment in MBRs will be crucial for the development of
appropriate biofouling control strategies in the future.

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 flow, but they have lower back transport velocity
due to lift forces in comparison to large particles (e.g., colloids
and sludge flocs). 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
filtration, 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
flocs. 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 figure out the detailed information on the
deposited biopolymers, identification 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 identification and characterisation of organic
fouling in MBRs. Through the FTIR spectra, the major
components of the biopolymers were identified 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
fluorescence analyses can help to conclude that membrane

1495

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 fluorescence
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 confirm that SMP
or EPS is the origin of organic fouling, and it plays significant
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 affinity with membranes.

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 filtration 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 filtration 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
ultrafiltration 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 significant
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
findings 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,

1496

water research 43 (2009) 14891512

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 biofilm 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
flux 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 significant 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 beneficial for the
membrane permeation in MBRs due to its positive effect on
sludge flocculation 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 efficiently remove inorganics on the

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

Chemical precipitation

COO-

COO

Biological precipitation

Mn+
COO-

Sludge flocs

Colloids

Solutes

Crystal

Fig. 6 Schematic illustration of the formation of inorganic

fouling in MBRs.

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 classified 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.

Bound EPS

3.1.1.

Definition of bound EPS and SMP

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
defined 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 unified 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 flocs 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

Bound EPS have been reported not only as major sludge floc
components keeping the floc 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 specific cake resistance and established a functional
equation in which the specific cake resistance was proportional to the EPS concentration. Ahmed et al. (2007) also

1497

water research 43 (2009) 14891512

Table 3 Relationship between various fouling factors and membrane fouling.

Sludge condition

Effect on membrane fouling

Ref.

- MLSS[ / normalized permeabilityY

- MLSS[ / fouling potential[
- MLSS[ / cake resistance[, specific cake resistanceY

(Trussell et al., 2007)

(Psoch and Schiewer, 2006a)
(Chang and Kim, 2005)

Viscosity

- Viscosity[ / membrane permeabilityY

- MLSS/Viscosity[ / membrane permeabilityY
- Viscosity[ / membrane resistance[

(Li et al., 2007a)

(Trussell et al., 2007)
(Chae et al., 2006)

F/M

- 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[

(Trussell et al., 2006)

(Watanabe et al., 2006)

Sludge condition
MLSS

(Kimura et al., 2005)

EPS

- polysaccharide[ / fouling rate[

- bound EPS influences on specific cake resistance
- polysaccharide[ / fouling rate[
- bound EPS[ / membrane resistance[
- The loosely bound EPS contributes to most of the
filtration resistance of the whole sludge

(Drews et al., 2006)

(Cho et al., 2005c)
(Lesjean et al., 2005)
(Chae et al., 2006)
(Ramesh et al., 2007)

SMP

- SMP is more important than MLSS

- colloidal TOC relates with permeate flux
- filtration 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

(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)

Filamentous bacteria

- filamentous bacteria[ / sludge viscosity[

- bulking sludge could cause a severe fouling
- filamentous bacteriaY / cake resistanceY

(Meng et al., 2007a)

(Sun et al., 2007)
(Kim and Jang, 2006)

- 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[

(Ahmed et al., 2007)

(Zhang et al., 2006b)
(Liang et al., 2007)
(Ng et al., 2006c)

HRT

- HRTY / membrane fouling[

- HRTY / membrane fouling[
- HRTY / membrane fouling[

(Meng et al., 2007a)

(Chae et al., 2006)
(Cho et al., 2005a)

Aeration

- aeration intensity[ / permeability[

- air-sparging improves membrane flux
- larger bubbles for fouling control are preferable
- air backwashing for fouling control is preferable
- bubble-induced shear reduces fouling significantly
- air scouring can prolong membrane operation

(Trussell et al., 2007)

(Psoch and Schiewer, 2006a)
(Phattaranawik et al., 2007)
(Chae et al., 2006)
(Wicaksana et al., 2006)
(Sofia et al., 2004)

Permeate flux

- sub-critical flux mitigates irremovable fouling

- sub-critical flux mitigates fouling

(Lebegue et al., 2008)

(Guo et al., 2007)

Operating condition
SRT

observed that as bound EPS concentration rose, the specific

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 influenced membrane fouling, and the
total biopolymers in sludge suspension played a more
important role than bound EPS in reflecting 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 flocculation 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 filterability could be observed.
Instead, the soluble EPS or SMP was found to have great
impact on the filterability of sludge. This was confirmed 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

1498

water research 43 (2009) 14891512

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, flocculation 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
efficiently.

3.1.3.

Behaviour and control of bound EPS in MBRs

According to literature, there is no efficient 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 finding 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 flocs 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 filtration (SRF)
values, which are used to characterise the sludge filterability,
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 benefit 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

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

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

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 flocs 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, filamentous bulking has been found to
have a strong influence on MBR fouling (Meng and Yang,
2007c; Su et al., 2007; Sun et al., 2007). The overgrowth of
filamentous bacteria leads to a sharp increase of bound EPS
concentration and then induces the increase of sludge
viscosity and sludge hydrophobicity. In addition, the filamentous bacteria can enlace and fix the foulants on the
membrane surface (see Fig. 8). Sun et al. (2007) observed that
with increasing sludge volume index (SVI), which results from
filamentous bulking, the average increasing rate of TMP
increased and the stable filtration period was shortened. Until
now, there are only a few studies about the cause and control
of filamentous bacteria in MBR processes, even though it

water research 43 (2009) 14891512

exhibits significant 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
filamentous bulking is to provide sufficient DO and alkalinity
for the sludge, because in many cases the filamentous 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.

SMP

3.2.1.

Effect of SMP on membrane fouling

In fact, fouling behaviour cannot be attributed solely to bound

EPS due to the complex nature of sludge suspension. Recently,
the influence 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 filterability of the sludge
suspension. Geng and Hall (2007) observed that the floc size
distribution and the amount of soluble EPS or SMP in the
mixed liquor were the most important properties that significantly influenced 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 significant membrane
foulant, scientific 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

1499

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 microfiltration 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 influence 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 significantly, and SMP concentration and
SMP composition would determine its fouling propensity.
Furthermore, the occurrence of SMP in MBR effluent 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)).

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 filtration
include inertial lift, shear-induced diffusion and Brownian
diffusion. It is difficult 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 filamentous bulking sludge.

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.

(Wisniewski and Grasmick, 1998)

(Defrance et al., 2000)
(Bouhabila et al., 2001)

20 days
40 days
60 days
SRT (Lee et al., 2003)

63
72
71
52
65
24

37
28
29
24
30
50

24
5
26

This study was tested in a cross-flow MBR.

TMP 100 kPa, u 3 m/s, T 15  C, SRT 60 d
MLSS 20.7 g/L, SRT 20 d

The sludge samples from lab-scale MBRs were filtered in a

batch test with a constant TMP of 27 kPa.

This study was performed in a batch filtration unit for 4 h

with a constant TMP of 4.0 kPa.
13
26
13
11
22
47
76
52
22
Bulking sludge
Normal sludge
Deflocculated
sludge
Sludge characteristics
(Meng and Yang, 2007c)

This study was performed in a cross-flow membrane

filtration cell for 5 h with a constant TMP of 100 kPa.
13
14
13
14
4
10
13
14
83
76
74
72
CA-1
CA-2
CA-3
CA-4
Membrane composition
(Bae and Tak, 2005b)

Solutes (%)
Colloids (%)
Flocs (%)

water research 43 (2009) 14891512

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

Remarks

1500

(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
influent 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 effluent increased to some
extent and then became stable, and finally 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 flat-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 flocs 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 flocculation 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 filterability 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 deflocculation of sludge flocs 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 sufficient supply of oxygen is
required in the bioreactor and sudden temperature change

water research 43 (2009) 14891512

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 influence on floc stability. Acetic acid
resulted in the production of high concentrations of small
particles (i.e., colloids and solutes) due to the weakly formed
flocs. Ethanol, on the other hand, encouraged the growth of
strong flocs 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
flocculation 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 bioflocs 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 floc breakage (Hu and Stuckey, 2007). Moreover,
the BAC flocs 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 fine colloids and solutes, and the
formation of a thin cake layer resulted in significant flux
improvement from 2 to 9 L/(m2 h). However, the addition of
3.4 g-PAC/L reduced the flux 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 flux significantly; 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 filamentous bacteria
and better flocculation, 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 filter 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
flocs) in the range of 110 mm. The improvement of membrane
flux or sludge filterability 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

1501

chain molecules, so that they had a better effect on filterability

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 flux enhancer (MFE), which is a modified 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 flocculation of activated sludge. SMP is
also entrapped by the microbial flocs during the course of the
flocculation, 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 flux
(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 flocs 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-flow
MBRs in scientific research and real applications, most of the
recent studies on hydrodynamic conditions are focused on the
reduction of aeration demand by enhancement of aeration
efficiency. In a cross-flow MBR, the membrane fouling can be
limited by increasing cross-flow 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 significant factor governing the filtration conditions.
Previous investigation (Han et al., 2005) showed that the cakeremoving efficiency of aeration did not increase proportionally with the increase in the airflow rate and that the airflow
rate had an optimum value from the cake-removing point of
view.

1502

water research 43 (2009) 14891512

Aeration is an important parameter determining both the

size of the sludge flocs and the membrane filtration or fouling
control. A high aeration rate certainly can reduce sludge
attachment to the membranes, but it also has a significant
influence on the biomass characteristics. Too high aeration
intensity will lead to breakage of sludge flocs 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 influence 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 flow rate play significant 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 efficient 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 airflow rates up to a given value
and beyond this flow rate no further enhancement was achieved (Ndinisa et al., 2006a). In addition, under certain conditions intermittent airflow can achieve better fouling control
than continuous filtration and it also reduces energy
requirements.
For submerged hollow fibers in bubble-enhanced systems,
such as the membrane bioreactor, the preferred fiber orientation should be vertical rather than horizontal though the
overall effect of fiber orientation on filtration is smaller than
the turbulence caused by the two-phase flow (Chang et al.,
2002b). The size of the gap between the submerged flat-sheet
membranes is also important for two-phase flow 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 flow decreased by at least 40%
based on suction pressure rise (dTMP/dt). Moreover, fiber
movement and fouling control are influenced by fiber tightness with significantly improved performance for slightly
loose fibers (Wicaksana et al., 2006). In recent years, to look for
a more efficient membrane fouling control, air-sparging in
MBRs has been paid more and more attention to (Delgado
et al., 2008; Psoch and Schiewer, 2008). The benefits of air-

sparging are the enhancement of hydrodynamic conditions

and the efficient use of aeration.
The interaction of two-phase flow with membranes in
MBRs is a complex issue. During the last few years, the analysis of the hydrodynamics and the fluid flow 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 flow 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 flat sheet MBR using twophase flow characterisation and CFD simulation. It was found
that the flux 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 influence 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
configuration, 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 field
(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 field, which could prevent the sludge flocs and
colloids depositing onto the membrane surface. In addition,
attempts also have been made to control MBR fouling by
developing novel filtration 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

water research 43 (2009) 14891512

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).

4.

Table 5 Summarization of fouling control strategies

based on various fouling factors.
Control
strategy

Control item and its effect on membrane

fouling factor

Hydraulic
control

- HRTY / sludge viscosity[ (Meng et al., 2007a),

EPS[ (Chae et al., 2006)
- aeration[ / permeability[ (Psoch and Schiewer,
2006a; Trussell et al., 2007), fiber movement[
(Wicaksana et al., 2006), cake-removing efficiency[
(Chang and Judd, 2003), and cake resistanceY (Psoch
and Schiewer, 2006b; Fan and Zhou, 2007)
- periodical backwashing / flux[ (Psoch and
Schiewer, 2006a) and operation period[
(Chae et al., 2006), total resistanceY (Psoch and
Schiewer, 2006b)
- sub-critical/low flux operation / sustainable
operation (Bacchin et al., 2006; Guglielmi et al.,
2007a)

Chemical
control

- 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)
- flocculation/coagulation / organic matterY
(Zhang et al., 2008c)
- chemically enhanced backwashing / remove
fouling (Kim et al., 2007)

Biological
control

- SRT[ / bound EPSY (Ahmed et al., 2007), SMPY

(Liang et al., 2007)
- MLSS/viscosityY / permeate flux[ (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)
- filamentous bacteriaY / bound EPSY (Meng et al.,
2006a)

Developments of membranes/filters

4.1.
Influence 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 fluoride (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 affinity between foulants (e.g., EPS/SMP)
and membrane. Zhang et al. (2008b) studied the affinity
between EPS and three polymeric ultrafiltration membranes,
and observed that the affinity 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 flux (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

1503

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 significant findings in membranes or filters used for MBRs.
The detailed discussion on the impacts of membrane material

Fig. 9 Favorable conditions mitigating membrane fouling.

1504

water research 43 (2009) 14891512

on membrane fouling can be found in recent reviews (Chang

et al., 2002a; Le-Clech et al., 2006).

4.2.

Application of low-cost filters

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 filters, which have small pores.
Since an improved effluent quality might not always be
required and only standard criteria are stipulated, it should be
feasible to substitute the membranes by cheaper filters with
large pore size. The low-cost filters investigated include (Ye
et al., 2006; Iversen et al., 2007; Seo et al., 2007; Satyawali and
Balakrishnan, 2008): non-wovens, meshes and filter cloths.
Non-wovens are composed of a random network of overlapping fibers having multiple connected pores through which
the fluid can flow (Chang et al., 2006). Due to its large pore size
or porosity, the non-woven could obtain a high-flux even at
very low pressure. There are little differences in the effluent
water quality between the non-woven bioreactor and the
membrane bioreactor (Meng et al., 2005). In 1998, non-woven
and coarse pore filter 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 efficiency was
91.6% producing an effluent COD concentration around
13 mg/L. These results confirmed 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 filter used in
wastewater treatment process, the non-woven still has its
own shortcomings. Compared with polymeric membranes,
some non-woven filters 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 filters,
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 flux 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 effluent 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 filtration of
activated sludge (Fan and Huang, 2002). As soon as the SFDM is
formed, it can improve effluent quality significantly. Besides
the low cost, it can be concluded that the high permeation at
very low suction pressure is another attractive character of
these filters.
The major problem limiting the application of low-cost
filters is the severe fouling due to their rough surface and the
too large pore size. The sludge flocs can entrap in the void
among the fiber matrix and it is difficult to be removed by
shear stress. Due to the large pore size, pore blocking by

sludge flocs is one of the main reasons leading to filter fouling

(Moghaddam et al., 2006). In order to avoid the rapid decline of
permeate flux of filter cloth, Ye et al. (2006) precoated the filter
cloth with powdered activated carbon (PAC) before
submerging it into a bioreactor. It was found that the precoated filter could not only mitigate membrane fouling, but
improve the effluent quality significantly as well. It indicates
that the severe fouling of low-cost filters can be resolved by
modifying the filters to improve the surface roughness,
hydrophilicity, surface charge and so on (see Section 4.3).

4.3.

Membrane modification

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 flux. To
improve the anti-fouling property of polypropylene hollow
fiber microporous membranes (PPHFMMs) in an MBR for
wastewater treatment, the PPHFMMs were subjected to surface
modification by NH3 and CO2 plasma treatment by Yu et al.
(2005a,b, 2008). The water contact angle reduced significantly
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 unmodified PPHFMMs. Although the
plasma treatment processes have many advantages, such as
a very shallow modification depth compared to other surface
modification techniques, it still has drawbacks. For example,
the chemical reactions of the plasma treatment are rather
complex, so the surface chemistry of the modified surface is
difficult 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 modification of polypropylene microporous
membranes was accomplished by UV irradiation in aqueous
acrylamide solutions. The contact angle data showed that the
hydrophilicity of the surface modified membranes increased
strongly with the increase of the grafting degree. Even though
the modified membrane showed better filtration ability in the
MBR than the unmodified 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 film on
the membrane surface, was employed for fabricating a fouling
resistance membrane in MBR (Asatekin et al., 2006). In this
study, commercial polyvinylidene fluoride ultrafiltration
membranes (PVDF UF) were coated with the amphiphilic graft
copolymer polyvinylidene fluoride-graft-polyoxyethylene
methacrylated (PVDF-g-POEM), to create thin film composite
nanofiltration membranes (TFC NF). The new TFC NF
membranes exhibited no irremovable fouling in 10-day deadend filtration 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

water research 43 (2009) 14891512

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 filtration 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 affinity 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-flow (Bae and Tak, 2005a,c). They
confirmed 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 filter by dip-coating PVA (polyvinyl alcohol). The
results obtained from two parallel MBRs indicated that the
flux decline of modified non-woven filter was only 12%, in
comparison of the original non-woven filter of 40%.
In addition to membrane modification, the development of
economical, high-flux, 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 firstly reported in 1965 by investigators at the Oak Ridge Laboratories engaged in desalination
research (Marcinko et al., 1966). Dynamic membranes can be
prepared by filtering 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 specific
components over the surface of a porous support. The selfforming membrane is formed by the components in the
solution to be filtered.
Many hydrated oxides, natural polyelectrolytes, and
synthetic organic polymers can be used for the preparation of
precoated membranes. It has been also reported that modified
membranes coated with an even PVA hydrogel layer show
dramatically high anti-fouling characteristics and good flux
recovery compared to inadequately modified membranes and
unmodified 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 firstly
reported by Li et al. (2005a), who prepared the dynamic

1505

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 influence 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 filter cloth with a pore size of
56 mm and powdered activated carbon were used as support
filter and precoating reagent. It was found that during the
long-term operation the removal efficiencies of organic
carbon and ammonia were as good as traditional hollow fiber
membrane bioreactors. The precoated filter cloth had a more
excellent performance with respect to fouling control than
uncoated filter cloth and hollow fiber membranes (Zhang
et al., 2005a). In addition, the precoated membrane had a low
irremovable fouling during the operation of MBRs. This finding
coincides with a previous study (de Amorim and Ramos, 2006).
It suggests that precoated dynamic membranes can help to
improve the filterability of filter cloths, mesh filters and nonwoven filters, so it provides these low-cost filters with a larger
potential in MBRs.
Self-forming dynamic membranes were firstly 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 flux and rejection of solutions.
The performance of self-forming dynamic membranes is
determined by concentration, type, shape, molecular weight
of filtering solution and cross-flow 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 filtration
reaches a steady state, a dynamic membrane will have been
formed, which mainly consists of large sludge flocs. 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 findings, 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 filters (i.e., filter 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

1506

water research 43 (2009) 14891512

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 classified into three major categories:
biofouling, organic fouling and inorganic fouling. The results
obtained from recent investigations on bound EPS, SMP, filamentous 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 identification 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 flux,
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 filtration 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 reflect 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, artificial 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 filters to substitute the membranes, modification
of membranes to enhance their hydrophilicity and use of
dynamic membranes to improve the performance of
membranes or low-cost filters. In the future, to our knowledge, the study on membrane materials in MBRs should still
focus on:
(1) Development of anti-fouling membranes or modification
of current membranes.
(2) Enhancement of the performance of low-cost filters by
modifying their surface properties.

Acknowledgements
The first 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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