Fouling in membrane bioreactors used in wastewater treatment

Pierre Le-Clech , Vicki Chen, Tony A.G. Fane

UNESCO Centre for Membrane Science and Technology, School of Chemical Engineering, The University of New South Wales,
Sydney 2052, NSW, Australia

Abstract
The membrane bioreactor (MBR) can no longer be considered as a novel process. This reliable and efficient technology has become a legitimate
alternative to conventional activated sludge processes and an option of choice for many domestic and industrial applications. However, membrane
fouling and its consequences in terms of plant maintenance and operating costs limit the widespread application of MBRs. To provide a better
understanding of the complex fouling mechanisms and propensities occurring in MBR processes, this review compiles and analyses more than
300 publications. This paper also proposes updated definitions of key parameters such as critical and sustainable flux, along with standard methods
to determine and measure the different fractions of the biomass. Although there is no clear consensus on the exact phenomena occurring on the
membrane interface during activated sludge filtration, many publications indicate that the extracellular polymeric substances (EPS) play a major
role during fouling formation. More precisely, the carbohydrate fraction from the soluble microbial product (also called soluble EPS or biomass
supernatant) has been often cited as the main factor affecting MBR fouling, although the role of the protein compounds in the fouling formation
is still to be clarified. Strategies to limit fouling include manipulating bioreactor conditions, adjusting hydrodynamics and flux and optimizing
module design.

Keywords: Membrane bioreactors; Fouling; Activated sludge; Operating conditions; Cleaning

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
1.1. MBR history . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
2. Fouling mechanisms for complex fluids . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
2.1. Concepts of critical and sustainable flux in mixed species environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
2.2. Effect of operating modes on performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
2.3. Cake structure and the effect of mixed species on cake morphology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
2.4. Effect of membrane morphology and surface chemistry on fouling mechanisms . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
2.5. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3. Roadmap for MBR fouling parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
3.1. Membrane characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
3.1.1. Physical parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
3.1.2. Chemical parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
3.2. Feedbiomass characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
3.2.1. Nature of feed and concentration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
3.2.2. Biomass fractionation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
3.2.3. Biomass (bulk) parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
3.2.4. Floc characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31

Corresponding author. Tel.: +61 2 93855762; fax: +61 2 93855966.

E-mail address: p.le-clech@unsw.edu.au (P. Le-Clech).
 3.2.5. Extracellular polymeric substances (EPS) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
3.2.6. Soluble microbial products (SMP) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
3.3. Operating conditions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
3.3.1. Aeration, crossflow velocity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
3.3.2. Solid retention time (SRT) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36
3.3.3. Unsteady state operation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37
3.4. Fouling mechanisms in MBRs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
3.4.1. Constant TMP operation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
3.4.2. Constant flux operation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
4. Mitigation of MBR fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
4.1. Removal of fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
4.1.1. Physical cleaning . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
4.1.2. Chemical cleaning . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
4.2. Limitation of fouling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42
4.2.1. Optimization of membrane characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42
4.2.2. Optimization of operating conditions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42
4.2.3. Modification of biomass characteristics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 44
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45

1. Introduction of the conventional activated sludge process was attractive, it

was difficult to justify the use of such a process because of the
Membrane bioreactor (MBR) technology combines the bio- high cost of membranes, low economic value of the product
logical degradation process by activated sludge with a direct (tertiary effluent) and the potential rapid loss of performance
solidliquid separation by membrane filtration. By using micro due to fouling. As a result, the focus was on the attainment of
or ultrafiltration membrane technology (with pore sizes ranging high fluxes, and it was therefore necessary to pump the mixed
from 0.05 to 0.4 m), MBR systems allow the complete physi- liquor suspended solids (MLSS) at high crossflow velocity at
cal retention of bacterial flocs and virtually all suspended solids significant energy penalty (of the order 10 kWh/m3 product) to
within the bioreactor. As a result, the MBR has many advan- reduce fouling. Due to the poor economics of the first gener-
tages over conventional wastewater treatment processes. These ation MBRs, they only found applications in niche areas with
include small footprint and reactor requirements, high effluent special needs like isolated trailer parks or ski resorts for exam-
quality, good disinfection capability, higher volumetric loading ple. The breakthrough for the MBR came in 1989 with the idea
and less sludge production [1]. As a result, the MBR process has of Yamamoto et al. to submerge the membranes in the biore-
now become an attractive option for the treatment and reuse of actor [6]. Until then, MBRs were designed with the separation
industrial and municipal wastewaters, as evidenced by their con- device located external to the reactor and relied on high trans-
stantly rising numbers and capacity. The current MBR market membrane pressure (TMP) to maintain filtration. The other key
has been estimated to value around US$ 216 million and to rise to steps in the recent MBR development were the acceptance of
US$ 363 million by 2010 [2]. However, the MBR filtration per- modest fluxes (25% or less of those in the first generation), and
formance inevitably decreases with filtration time. This is due to the idea to use two-phase bubbly flow to control fouling. The
the deposition of soluble and particulate materials onto and into lower operating cost obtained with the submerged configuration
the membrane, attributed to the interactions between activated along with the steady decrease in the membrane cost encouraged
sludge components and the membrane. This major drawback and an exponential increase in MBR plant installations from the mid
process limitation has been under investigation since the early 1990s. Since then, further improvements in the MBR design
MBRs, and remains one of the most challenging issues facing and operation have been introduced and incorporated into larger
further MBR development [3]. plants. While early MBRs were operated at solid retention times
(SRT) as high as 100 days with mixed liquor suspended solids
1.1. MBR history up to 30 g/l, the recent trend is to apply a lower SRT (around
1020 days), resulting in more manageable mixed liquor sus-
The MBR process was introduced by the late 1960s, as pended solids (MLSS) levels (1015 g/l). Thanks to these new
soon as commercial scale ultrafiltration (UF) and microfiltra- operating conditions, the fouling propensity in the MBR has
tion (MF) membranes were available. The original process was tended to decrease and overall maintenance has been simplified
introduced by Dorr-Olivier Inc. and combined the use of an as less frequent membrane cleaning is necessary. There is now a
activated sludge bioreactor with a crossflow membrane filtra- range of MBR systems commercially available, most of which
tion loop [4]. The flat sheet membranes used in this process use submerged membranes although some external modules are
were polymeric and featured pore size ranging from 0.003 to available; these external systems also use two-phase flow for
0.01 m [5]. Although the idea of replacing the settling tank fouling control. In terms of membrane configurations, mainly
hollow fiber and flat sheet membranes are applied for MBR
applications [7].
The economic viability of the current generation of MBRs
depends on the achievable permeate flux, mainly controlled
by effective fouling control with modest energy input (typi-
cally 1 kWh/m3 product). More efficient fouling mitigation
methods can be implemented only when the phenomena occur-
ring at the membrane surface are fully understood. The plethora
of publications dealing with MBR fouling and published within
the last 5 years tends to dilute the accessibility of informa-
tion and may lead to some confusion. This review presents
a state-of-the-art assessment of MBR fouling based on the
most recent and relevant papers on the subject. After discus-
sion of fouling mechanisms for complex fluids, a comprehensive
roadmap for MBR foulants and fouling parameters will be pro-
posed. Finally, a review of the current methods for fouling
mitigation in MBR systems will detail design options to opti-
mize MBR operation. This review aims to open doors to new
ideas and directions for optimized and more sustainable MBR
processes.

2. Fouling mechanisms for complex uids

Significant advances in understanding fouling of individual

components such as bacteria, yeast, proteins, and colloids have
occurred in microfiltration and ultrafiltration literature [811].
Much of this literature has focused on the effect of charge (via pH
variation or salt concentration), crossflow, concentration, mem-
brane hydrophilicity, membrane pore size and flux (constant
pressure or constant flux). While some broad trends for simple
colloids are valid for macromolecules (the most commonly stud-
ied of which are proteins), the labile nature of proteins and range
of polydispersity of naturally occurring macromolecules such
as polysaccharides and humic substances add a particular com-
plexity to the fouling mechanisms. In addition, the interaction
between the suspended colloids or those in the deposited cake
in a mixed species environment has the potential to significantly
change the nature of the foulant layer in terms of resistance and
reversibility, even for simple model systems. In this section, the
heuristics providing insights to fouling in such mixed species
environment are considered in the context of broad observations
and commonly used tools to decipher them.
2.1. Concepts of critical and sustainable ux in mixed
species environment
Optimizing flux to control fouling has been pursued since
the mid-1980s. Moderating TMP differences within modules
had been utilized to reduce excessive localized fouling. While
much of the existing literature has been performed under con-
stant pressure conditions, the use of constant flux and monitoring
of resultant TMP rise have proved to be particularly useful in
the context of monitoring fouling in complex fluids and is cur-
rently the mode of choice in many MBR applications (Fig. 1).
Typically, increasing flux steps are imposed and the TMP mon-
itored for its stability at each step. When the TMP is no longer
stable at each flux step and increases rapidly to indicate rapid
Fig. 1. (a) Critical flux determination by the flux-stepping method and (b)
resulting data obtained during the study of the effect of membrane state (BW:
backwashed, chemically cleaned or new) on the fouling rate (dP/dt) [14].
accumulation of foulants, this is usually referred to as the crit-
ical flux. The original critical flux hypothesis for MF assumes
that a critical flux exists below which a decline of permeability
with time does not occur, and above which fouling is observed
[12]. Since this first definition, the critical flux concept has been
refined with numerous different meanings, definitions and meth-
ods of determination, reviewed in [13,14]. Two distinct forms of
the critical flux concept have been defined, with, respectively,
no fouling and little fouling occurring at sub-critical operation
for the strong and weak forms. In practice, the flux obtained
during sub-critical flux (strong form) equates to the clean water
flux obtained under the same conditions. In the alternative weak
form, the sub-critical flux is the flux rapidly established and
maintained during the start-up of the filtration, but does not nec-
essarily equate to the clean water flux.
The critical flux depends on the back transport provided by the
crossflow or turbulence generated by imposed liquid flow and/or
bubbling as well as the specific solutemembrane interactions,
which are affected by charge and hydrophobicity. Solute size
also plays a significant role in determining the regime of back
transport whether it is diffusive or inertial lift [8]. High local
concentrations that promote local aggregation due to concen-
tration polarization will also determine the cohesiveness of the
foulant layer.
 For single particles, the force balance between convective
drag to the membrane and back transport due to crossflow can be
analyzed with various shear enhanced diffusivity models [15] to
predict the critical flux at which deposition occurs at a particular
hydrodynamic condition. The reversibility of the deposition has
been less well documented but can be assessed by examining the
hysteresis of the TMP versus flux profile [16,17]. The hysteresis
technique is the most recently formalized technique to deter-
mine critical flux. By using this method, Chen et al. [16] studied
the transition from concentration polarization to cake forma-
tion during the membrane filtration of colloidal silica. Recently,
Espinasse et al. [18] published a proposed standard method for
the determination of critical flux using hysteresis effects. In this
method, critical flux is defined as the lowest flux that creates
an irreversible deposit on the membrane. Models proposed by
Bacchin and co-workers [1921] to incorporate intermolecu-
lar forces with convective transport have been used to predict
regimes where particle aggregation begins to dominate on the
membrane surface.
For macromolecules, the apparent critical flux can also be
determined however in these systems, background adsorption
occurs even with no convection and a slow increase in mem-
brane resistance is always detected even at low fluxes. The
kinetics of this adsorption, particularly for proteins, can be cru-
cial as conformational changes of the initial adsorbed layer can
change the surface chemistry of the membrane surface with
time. This continual adsorption may close off smaller pores
that cause redistribution of flow throughout membrane structure.
While concentration polarization may not be initially present
for these small macromolecules in microfiltration, the adsorp-
tion followed by retention of an increasing fraction of the feed
can result in rapid loss in transmission and resultant polariza-
tion. High initial flux (typical of constant pressure experiments)
can also generate aggregation of some macromolecules such as
proteins [22,23].
For complex uid systems, one common practice to exper-
imentally determine the critical flux value is to incrementally
increase the flux for a fixed duration. This leads to relatively
stable TMP at low fluxes (indicating little fouling), and an ever-
increasing rate of TMP rises at fluxes beyond the critical flux
values [16,2428]. Since zero rate of TMP increase is generally
not attained in filtration of complex fluids, no critical flux, in its
strictest (or strong) definition, can be defined (Fig. 1). In fluids
with both macromolecules and particulates, membrane fouling
takes place even at low flux rates, but changes dramatically when
the so-called critical flux (in its weak form) is reached. Although
apparently straightforward in principle, the precise identifica-
tion of the critical flux value from flux-stepping experiments
strongly depends upon the conditions used (step duration, step
height, initial state of the membrane) [14]. The most important
parameter remains the step height, which needs to be kept as
small as possible for higher accuracy in the determination of
the critical flux value [13]. Unfortunately, no standard protocol
exists, such that the comparison of critical flux values reported in
the literature is difficult. The determination of the exact value of
the critical flux (i.e. the passage from little to severe fouling) is
then left to the judgement of the researchers, although rigorous
mathematical expressions have been reported [14]. In spite of the
arbitrary aspect of this method, critical flux determination by this
short-term experiment remains an efficient approach to assess
the fouling behavior of a given filtration system and to compare
different operating conditions. Interestingly, this method was
recently used as a standard test to assess the fouling propen-
sity of an MBR on a daily basis [29]. This approach allows the
plotting of fouling intensity against an MBR parameter such as
biomass characteristics.
It is also now generally accepted that the short-term determi-
nation methods for the critical flux (especially the flux-stepping
approach) does not yield predictive absolute permeability data
for extended operation of complex fluids. For example, the foul-
ing rate (dTMP/dt) values measured for long-term experiments
are always significantly lower than the equivalent values mea-
sured for the short-term flux-step experiments [13,14,3032].
In addition, a second phase of TMP increase has been observed
when long-term filtration was carried out at sub-critical flux
(experimentally determined in short-term experiments) even for
simple model feeds, such as alginate solutions. A number of
models have been proposed to account for the development of
a second phase of TMP increase which may occur after hun-
dreds of hours of operation [17,31,33,34]. Most of the models
have focused on the potential for slow pore closure or blockage
that results in high local fluxes due to redistribution of flow and
subsequent rapid fouling.
The challenge remains to use short-term experimental data to
project long-term fouling characteristics in such mixed systems
where foulant inventory and fractionation may play important
roles. Thus the focus may be shifted to considering a sustain-
able flux (see Section 4.2.2) where reversibility of the foulant
deposition and global operational constraints for productivity
and costs are taken into account.
2.2. Effect of operating modes on performance
Constant pressure filtration behavior is typified by a rapid
flux decline at the start of filtration followed by a more grad-
ual decrease until a steady-state or a pseudo-steady-state flux is
reached. Four filtration models (Table 1), originally developed
for dead-end filtration [35], have been proposed to describe the
initial flux decline.
Comparison between operating modes (constant pressure and
constant flux) have been limited [27,36,37]. Constant flux oper-
ation avoids excessive fouling of membranes as well as being
cost effective for submerged membrane operations [27]. Vyas et
al. [38] investigated the performance of different combinations
of constant pressure and constant flux crossflow microfiltration
of lactalbumin suspensions, since in their case the critical flux
is too low to be an economic operation. It was found that oper-
ating under constant flux just above the critical flux followed
by constant TMP operation causes severe membrane fouling.
It appears that during the constant TMP period, small parti-
cles continued to permeate through the relatively thinner cake,
formed during the low constant flux filtration, into the mem-
brane pores. In contrast, constant TMP operation followed by
very low constant flux operation can offer scope to reduce
Table 1
Empirical dead-end filtration equations
Law Physical cause Description Equation

Cake filtration
Complete blocking
Intermediate blocking
Standard blocking
Boundary layer resistance
Pore blocking
Long-term adsorption
Direct adsorption
Deposit of particles larger than the membrane pore size onto the t/V = AV + B
membrane surface
Occlusion of pores by particles with no particle superimposition ln(J/J0 ) = At + B
Occlusion of pores by particles with particle superimposition 1/J = At + B
Deposit of particles smaller than the membrane pore size onto the t/V = At + B
pore walls, reducing the pore size

Where V is the cumulative volume of permeate at time t, J the flux, and J0 is the initial flux.

surface fouling by reducing the convective force towards the
membrane.
While fouling is generally observed as being slower in con-
stant flux operation, there is some evidence that the deposition
under these low fouling conditions may be more irreversible as
the resultant mechanism tends to be predominately internal foul-
ing by macromolecular species. Constant flux operation may
generate a substantial initial deposit, but its effect on subse-
quent deposition of macromolecules may be beneficial in some
circumstances by serving as a prefilter for species which may
otherwise infiltrate more deeply into the membrane pores. In
addition, the constraints of productivity in terms of flux and per-
meation of targeted species for applications such as fermentation
redefine the optimal flux operational mode.
Intermittent filtration combined with continuous crossflow
may allow deposits to relax as long as the particles are still labile.
In appropriate regions suggested by Bacchin et al. [19] where
coagulation or aggregation has not occurred, this approach may
allow removal of foulant cakes. However, for many biological
solids, the cohesive strength of the cake may be significant and
proteins adsorption and gel formation result in strong attractive
bonds to the membrane materials.
2.3. Cake structure and the effect of mixed species on cake
morphology
Once the cake is formed on the membrane surface, the cake
layer offers an additional resistance for filtration. The perme-
ability of the cake layer can be affected by flux, electrostatic
interactions, and particle size. General observations by Petsev
et al. [39] include:
When salts do not cause aggregation in the feed, the perme-
ability of the cake layer sharply decreases with the increase
in electrolyte concentration.
The permeability of the cake layer sharply decreases with the
increase in permeate flux because the increased flux results in
a more compressed cake layer.
The permeability of the cake layer increases with the surface
potential of the particles due to the increase in the inter-
particle repulsion. However, above a certain value of surface
potential, a plateau value for the permeability is reached.
The permeability of the cake layer passes through a minimum
with the increase in the particle size.
The reason for such behavior is that for very small parti-
cles, inter-particle repulsion (electrostatic repulsion) exerts a
dominant effect on the voidage of the cake layer. In this range
of particle size, the inter-particle repulsion decreases with the
increase in particle size resulting in the decrease of permeability
[40]. After a certain value of particle size, the effect of the elec-
trostatic force becomes negligible and the permeability increases
with the increase in particle size. Fane et al. [41] observed a
similar dependency of the permeability of the cake layer on
particle size. They proposed a different explanation based on
the counter balance of the Brownian diffusion (dominating for
smaller particles) and particle migration due to hydrodynamic
forces (dominating for larger particles).
The development of the cake layer during microfiltration
was also studied [4247]. Cakes formed in the crossflow mode
may have higher specific cake resistances than cakes formed in
dead-end filtration and may even increase with the increase in
membrane resistance [48]. Many of these observations can be
explained by size dependent particle deposition and the depen-
dence of the specific resistance on the particle size. Based on the
mass transfer mechanisms, there is a maximum diameter of par-
ticle that can deposit on the membrane surface. As the crossflow
velocity increases, the cut-off diameter decreases, allowing that
smaller particles to deposit on the membrane surface. Thus spe-
cific resistance may increase. In addition, cake formation during
crossflow tends to eliminate larger particles from the deposits,
leading to cake containing a finer fraction of the particle size
distribution. Plugging and catastrophic reduction in permeabil-
ity of the retained cake is another potential cause of the two
stage TMP increase during sub-critical flux operation indicated
earlier [34]. However, Keskinler et al. [44] reported that the spe-
cific resistance for lower crossflow velocities was greater than
the one obtained in higher crossflow velocities for all yeast cell
concentrations tested. In contrast, during the membrane filtra-
tion of monodisperse latex particles, no effect of stirring speed
was found on the specific resistance values [43].
The compressibility indexes of the cake have been found to
be different in crossflow and dead-end filtration. Keskinler et al.
[44] found that non-living yeast cakes formed in the crossflow
mode are more compressible than cakes formed in dead-end
filtration. The compressibility index was found to be 1 and
0.39 for the crossflow and dead-end filtration, respectively.
Xujiang et al. [49] found similar trends during microfiltration
of talc suspensions. By contrast, Mota et al. [50] reported that,
for spherical particles, the compressibility index (n) both in
dead-end and crossflow filtration were similar basing on the
studies at relatively low crossflow velocity. Tanaka et al. [45]
found lower compressibility index in crossflow filtration than
that in dead-end filtration during microfiltration of rod-shaped
B. subtilis, which are 0.6 and 0.8, respectively. They explained
these differences as follows. During the crossflow filtration
at lower TMP, the cells were arranged by the shear from the
beginning of cell deposition on the membrane surface, thus the
cake showed higher specific cake resistance than that in the
dead-end filtration. While at higher TMP, the cells deposition
at the initial stage of crossflow filtration in particular tended to
deposit in a manner similar to that in dead-end filtration due to
the high permeate flux; therefore the specific cake resistance
became close to that in the dead-end filtration. This may provide
the reason that the compressibility is lower in crossflow filtration
than dead-end filtration. Hughes and Field [51] recently showed
that increasing shear stress reduced the amount of reversible
fouling in yeast filtration but the irreversible component
remained constant. The potential for size segregation and lateral
transport for yeast cells near the membrane wall has also been
observed [52]. Foley [53] recently reviewed factors affecting
filter cake properties of microbial suspensions.
For complex fluids such as membrane bioreactors effluent,
fermentation broths, and natural organic matter, the fouling
interactions of the colloidal component are affected by the poten-
tial for small macromolecules to penetrate and adsorb into the
membrane structure and foulant cake structure. On the other
hand, colloids or particles can affect the initial deposition of the
macromolecules by adsorbing them on their surfaces or provid-
ing a secondary layer that entraps aggregates of these macro-
molecules. Studies to elucidate this phenomenon have been
carried with yeast and protein mixtures. Davis and colleagues
[5456] showed that the presence of yeast actually prevented
fouling of bovin serum albumin (BSA) in microfiltration as the
yeast layer on the membrane surface captured the BSA aggre-
gates and prevented them from fouling the internal structure of
the membrane. In this case, the cake layer formed by the yeast
particles can be considered as a prefilter (Fig. 2). They observed
higher protein transmission and higher flux in the presence of
the yeast cake than in its absence. Recent studies by Ye and
Chen [57] showed that the critical flux of the mixtures of yeast
and BSA showed little change from critical flux measured for
yeast alone; however, the reversibility of the deposited formed
by these mixed layer is substantially reduced. Thus the macro-
molecules can serve to bind the particulates together. Results
Fig. 2. Cake layer as prefilter.
with alginate, a microbial polysaccharide, showed increasing
specific resistance with time, indicating a consolidation of the
cake layer formed which may be due to infiltration of small
fractions of the alginates among the alginate aggregates initially
trapped by the microfilter. When both alginate and protein are
present, the transmission of both components was reduced while
the compressibility of the mixed deposit was increased. Thus the
rigidity and compressibility may vary substantially depending
on the chemical nature of the extracellular components bound
or soluble in MBR or fermentation broths.
Some researchers indicated that particles in the mixed feed
solution determine the flux behavior during the membrane fil-
tration. Timmer et al. [58] found that the small quantities of
silicates completely determined the flux behavior in the cross-
flow microfiltration of -lactoglobulin solutions. Causserand et
al. [59] studied the permeability changes in clay cake due to
protein adsorption. A minimum limiting flux was found at the
isoelectric point of the clayprotein complex. Interestingly, they
found that at higher pH values, the mixture behavior was simi-
lar to the protein, whereas below pH 4.5, the limiting flux was
similar to those observed for the filtration of clay suspensions
alone. By optimizing the electrostatic interactions between pro-
teins and an adsorptive surface like clay, Causserand et al. [60]
improved protein fractionation and decreased membrane foul-
ing by the protein, which was attributed to the formation of a
secondary membrane by clay particles on top of the original par-
ticles. Hwang et al. also showed that capture of BSA in bed of
latex particles can be related by standard capture equation for
deep-bed filtration. Interesting studies by van Oers et al. showed
how the presence of silica sols can reduce rejection of polyethy-
lene glycol (PEG) and dextran by providing a high polarization
layer (unstirred) zone near the membrane [61]. In contrast, the
rejection of PEG and dextran increased in the presence of BSA.
The compressibility of the BSA layer leads to highest rejection
occurring at the highest pressure of filtration.
The impact of large particles on the fouling process is not easy
to gauge. Researchers have indicated that fouling can be reduced
by adding suspended solids during UF of organic molecules
such as polysaccharides and proteins. Panpanit and Visvanathan
[62] investigated the role of bentonite addition in the UF for
oil/water emulsions. It was found that the addition of ben-
tonite up to a certain concentration dramatically decreased the
membrane fouling. This was because the reduction of oil/water
emulsions concentration by bentonite adsorption and the forma-
tion of larger particles when oil/water emulsion contacted with
bentonite. However, beyond the limiting concentration, the flux
improvement gradually declined, possibly due to the formation
of packed cake of particles on the membrane surface. This com-
posite cake structure is illustrated in Fig. 3. Recent studies with
bentonite and alginate mixtures during constant flux MF showed
formation of a bentonite cake near the membrane while the algi-
nate formed a viscous layer above the cake. Particle velocities
through this viscous layer dropped steadily as filtration time pro-
ceeded, indicating densification of the viscous gel layer (Fig. 4).
This may provide insight into the cohesive and transport charac-
teristics of such composite layers. In contrast, compact cellular
or particulate cakes which form with swollen macromolecular

Fig. 3. Composite cake structure.
underlayer may disengage spontaneously if the cake build-up is
sufficient to create high shear stress due to crossflow [63].
In systems with the microorganisms, the likelihood of dif-
ferent cell wall properties precluded researchers from making
definitive statements regarding the effects of cell size and shape
on filtration characteristics. In this context, Foley and his co-
workers used polymorphic microorganisms to conduct a detailed
investigation of the effect of cell size and shape on filtration
behavior [48,6467]. The shape of this microorganism, ranging
from yeast-like to filamentous, could be varied in a controlled
way by altering its growth conditions. The structure of the cell
wall was reasonably constant and independent of the cell shape.
The results clearly showed that the specific cake resistance
and compressibility of the microbial filter cakes was strongly
related to cell morphology, in particular the mean aspect ratio
of the cells. The potential errors in calculating specific resis-
tance and tortuosity is significant in mixed species cakes and
the effect of cell shapes and structure in a compressible media
may require better understanding of the associated extracellular
material [50,68].
Recent work by Ohmori and Glatz [69] and earlier work by
Hodgson et al. [68] have shown that the filtration properties of
microbial suspensions were dependent not only on the cell shape
but also on the physical characteristic of the cell and associated
extracellular matrix. Ohmori and Glatz [69] found that changes
Fig. 4. Velocity profile during filtration of binary model solution with direct
observation apparatus (500 mg/l alginate50 mg/l bentonite solution; apparent
bulk velocity = 2 mm/s; constant flux of 56 l/m2 h). The background picture
shows the fouling layer after 2 h of filtration.
in carbon source for the fermentation of C. glutamicum affected
the microfiltration performance. The specific cake resistance of
cells cultivated with sucrose was half as much as those culti-
vated with glucose at neutral pH, and were almost the same
below pH 4.0. The authors attributed these differences in spe-
cific cake resistance, as well as their pH dependencies, to the
higher hydrophobicity and lower surface charge of cells grown
on sucrose. By performing extracellular matrix modification of
marine bacteria SW8 with a proteolytic enzyme and a chelating
agent, the important role of matrix in resistance was confirmed
by the changes of flux and specific cake resistance [68].
2.4. Effect of membrane morphology and surface chemistry
on fouling mechanisms
Conventional wisdom generally attributes lower fouling to
smooth hydrophilic membranes with high porosity and narrow
pore size distribution. This has been supported by extensive work
with various biological fluids, particularly proteins solutions
[10,11,70,71]. Reduction in the macromolecular adsorption with
hydrophilic surfaces or by mitigating charge interactions will
reduce the rate of pore closure due to this mechanism. Met-
samuuronen et al. [72] reported that much lower critical fluxes
were observed for the ultrafiltration of bakers yeast when a
hydrophobic polysulfone membrane was used as opposed to a
hydrophilic regenerated cellulose membrane. This phenomenon
is more obvious at pH 6 where both membranes have a zeta
potential of zero. By using matrix-assisted laser desorption ion-
ization mass spectrometry (MALDI-MS) for quantitative analy-
sis, Chan et al. [73] studied the membrane fouling by protein
mixtures on hydrophilic and hydrophobic 30 kDa molecular
weight cut-off (MWCO) UF membranes. It was found that, for
the hydrophobic membrane, the deposition exceeded quantities
corresponding to a monolayer above and below the apparent
critical flux. When a hydrophilic membrane was employed,
coverage in excess of a monolayer was only found above the
apparent critical flux. Interestingly, while high molecular weight
proteins appear to dominate the apparent critical flux, the pre-
dominant proteins observed on the membrane by this technique
tended to be the lower molecular weight species [74] that pene-
trate the pores. In mixed species feeds, the surface chemistry of
the membrane may be masked by adsorption of the multitudes
of macromolecular species thus the benefits of hydrophilicity
may be obscured during the long-term fouling.
At a given fixed flux, one would initially expect the pore size
of the membrane to be irrelevant to the convective force exerted
on the particles and to any back diffusion or shear induced
diffusion effect. However, as pore size decreases, hindered trans-
port of macromolecules exacerbates local polarization and the
potential for aggregation and fouling. The local porosity and
associated local convective velocities as opposed to average flux
across the whole membrane surface also need to be considered
when comparing membranes with widely varying porosities.
The influences of pore size on the fouling were found to dif-
fer in various studies. In the microfiltration of 0.4 wt.% BSA
solutions, Chen [75] found that the critical flux increased with
pore size when track-etched membranes of pore size 0.1, 0.2 and
0.4 m were used. In comparison, Wu et al. [76] investigated the
effect of membrane pore size (50 kDa, 100 kDa and 0.2 m) on
critical flux for three types of feed fluids. For all feed fluids
tested: 0.5% silica, 0.15% BSA and 5% yeast cell suspension,
the critical flux decreased with increasing membrane pore size.
Narrow pore size distributions reduce the inhomogeneous
flow distribution between pores that lead to preferential deposi-
tion and blockage of large pores [77,78]. Similarly, high porosity
means that local flux at the pore entrance will be reduced. Mem-
branes with interconnecting pore structures also have the advan-
tage that surface blockage can be mitigated [79]. Membrane
morphology will determine initial macromolecular transmission
and fouling mechanisms, particularly at low flux operation. The
transition between pore closure and cake formation is critical in
the fouling progression in mixed species feed. As the effective
pore size is reduced, the local flux increases, increasing the con-
vective forces to the pore. Larger particles are then pulled in and
accelerate the foulant build-up.
Typically, membrane blocking laws (constant flux and con-
stant pressure mode) have been used to establish when this
transition between pore blockage and cake formation takes place
[80]. Ho and Zydney [81] have developed a combined pore
Fig. 5. Progressive pore blockage leading to rapid TMP increase.
blockage and cake formation model, with the cake layer only
forming over the regions of the membrane that have already been
blocked by the initial deposit in the membrane pores. Unlike
most prior pore blockage models, it was assumed that some
3. Roadmap for MBR fouling parameters
fluid is still allowed to flow through the pores blocked by large
aggregates. The model was successfully used to analyze the pro-
All the parameters involved in the design and operation of
tein fouling [81], alginate fouling [33] and humic acid fouling
MBR processes have an influence on membrane fouling. For the
[82] during microfiltration.
purpose of this review, three categories of factors are defined, i.e.
membrane and module characteristics, feed and biomass param-
2.5. Summary
eters and operating conditions (Fig. 6). While some of these
parameters have a direct influence on MBR fouling, many others
In complex fluids, the interactions between the macromolec-
result in subsequent effects on phenomena exacerbating fouling
ular and particulate components of the feed can result in unex-
propensity. The complex interactions between these parameters
pected and rapid changes in fouling. The kinetics and inventory
complicate the perception of MBR fouling and it is therefore
of macromolecules adsorbing will dictate the initial fouling
crucial to fully understand the biological, chemical and physical
phase. Progressive closure of pores or membrane surface results
phenomena occurring in MBRs to assess fouling propensity and
in a change in transmission and species convected to the surface
mechanisms.
and the foulant cake. While the initial low fouling phase at low
flux (or sub-critical flux) features slow progressive adsorption
of macromolecules on the membrane surface, a more rapid foul-
ing phase then occurs. During that period, pore closure results in
enhanced rejection of macromolecules and deposition of larger
particles (Fig. 5). Evolution of this foulant cake and its irre-
versibility depend on both its composition and the hydrodynamic
environment under which it was established. The interaction
between particulate and macromolecular fouling needs to be
considered with many of the same complexities observed in
fouling studies of natural organic matter. Macromolecular foul-
ing can increase particulate adhesion, but particles can affect
the transmission and infiltration of macromolecules into the
membrane pores. Greater understanding of the foulant struc-
ture in mixed specie systems will allow better control measures
to prevent foulant build-up or to disengage the foulant layer. The
lessons learnt from such studies are important for understanding
fouling in MBRs. Fig. 6. Factors affecting fouling in submerged MBRs.
3.1. Membrane characteristics
3.1.1. Physical parameters
3.1.1.1. Pore size and distribution. The effects of pore size (and
distribution of pore size) on membrane fouling are strongly
related to the feed solution characteristics and in particular
the particle size distribution. Depending of the pore size and
the type of biomass filtered, results reported in the literature
have shown opposite trends. If particle size is smaller than
pore size, pore blocking and/or restriction is expected. It is
therefore expected that large pore membranes like MF would
present higher fouling propensity compared to UF membranes.
Table 2 reports results obtained in 11 studies during which
the pore size effects have been assessed by different fouling
parameters. It is quite clear from this table that the pore size
alone cannot predict hydraulic performances as no general trend
was observed between these two parameters. The complex and
changing nature of the biological suspension present in MBR
systems and the large pore size distribution of the membrane
generally used in MBR are the main reasons for the unde-
fined general dependency of the flux propensity on pore size
[83,84]. Additionally, the duration of the experiment and other
operating parameters like crossflow velocity (CFV) and con-
stant pressure or constant flux operation have a direct influ-
ence on the determination of the optimization of the membrane
pore size (Table 2). For example, when MF and UF mem-
branes were compared in a similar environment (with a CFV
of 0.1 m/s), the MF membrane produced a hydraulic resistance
around twice that of the UF membrane. In that same study, the
fouling behaviors of the MF and UF membranes were differ-
ent when operated at higher CFV. This was due to the effect
of CFV on critical flux of particulates (Section 3.3.1). Inter-
estingly, the dissolved organic carbon (DOC) rejection of both
membranes were similar after 2 h of operation, indicating the
creation of a dynamic membrane layer on the MF membrane
[85].
The long-term effect of UF membrane pore size on hydraulic
performances has been assessed by He et al. for anaerobic MBR
operated under constant TMP [87]. The smallest MWCO tested
(20 kDa) featured the largest permeability lost within the first
15 min of filtration when compared to 30, 50 and 70 kDa mem-
branes. However, when operated for extended time (over 100
days) with regular hydraulic and chemical cleaning, the largest
MWCO membrane (70 kDa) experienced the greater fouling
rate, as 94% of its original permeability was lost, compared to
only 70% performance decrease for the other three membranes.
As a result, the 30 and 50 kDa membranes provided the best
overall hydraulic performances, indicating the possibility of an
optimum membrane pore size for a given application and for a
given filtration time. These results also revealed that the experi-
ment duration is crucial to fully assess the fouling propensity of
a membrane. Similar trends showing the time dependency for
large pore MF with the highest initial fouling for the smaller
pore and the greater long-term fouling for the larger pore were
reported for pore size ranging from 1.5 to 5 m operated at con-
stant TMP [90]. While the quest for the highest steady-state
permeability is probably desirable, it is important to be aware
that conclusions derived from flux decline data could be some-
times deceptive, as an intrinsically high flux membrane may
appear to foul more for the same increment of resistance.
It is expected that smaller pore membranes would reject a
wider range of materials, and the resulting cake layer features a
higher resistance compared to large pore membranes. However,
this type of fouling is more reversible and is easily removed dur-
ing the maintenance cleaning than fouling due to internal pore
clogging obtained in larger pore membrane systems. The irre-
versible fouling, due to the deposition of organic and inorganic
materials onto and into the membrane pores is the main cause
of the poor long-term performances of larger pore size mem-
branes. However, when testing membranes with pores ranging
from 0.4 to 5 m (at constant TMP), Gander et al. observed
the opposite results, i.e. higher initial fouling for large pore and

Table 2
Effect of pore size on MBR hydraulic performances
Membranes tested Optimum Test duration Other References

0.1,0.22, 0.45 m 0.22 m 20 h [86]a

70 kDa 110 min High concentrated
20, 30, 50, 70 kDa [87]
50 kDa 110 days Feed, anaerobic
70 kDa, 0.3 m 70 kDa 8h [88]
30 kDa 2h CFV = 0.1 m/s
30 kDa, 0.3 m [85]
0.3 m Merge CFV = 3.5 m/s
0.1, 0.2, 0.4, 0.8 m 0.8 m n/a [89]a
200 kDa, 0.1, 1 m 1 m 3h Based on critical flux test [84]a
5 m 25 min [90]
0.3, 1.5, 3, 5 m
0.3 m 45 days
0.4 m 1 day [91]
0.4, 5 m
No effect From 50 days
0.01, 0.2, 1 m No effect Few hours Based on critical flux test [92]a
200 kDa, 0.1, 1 m 0.1 m n/a Anaerobic [93]
0.05, 0.4 m 0.05 m n/a [94]
a Constant flux operation, non-marked references are constant TMP operation.
significant flux decline when the small pore membrane was used
over an extended period of time [91] (Table 2). Characterization
of the molecular weight (MW) distribution of the compounds
present in the supernatant of MBRs operated with four pore sizes
(ranging from 0.1 to 0.8 m) has also been presented [89]. With
apparent lower fouling rate, the 0.8 m pore size MBR featured
a slightly higher concentration of most of the macromolecules
present in the bioreactor supernatant. However, it seems unlikely
that the small differences in MW distribution are the main cause
of the various fouling rates observed between the four MBR
systems.
In another study based on short-term experiments, sub-
critical fouling resistances and fouling rates increased linearly
for membrane resistances ranging from 0.4 to 3.5 1011 m1 , design tends to favor submerged over sidestream configurations
corresponding to membrane pore size from 1 down to 0.01 m,
respectively [84]. These results indicated the creation of a
dynamic layer of greater overall resistance for more selective
membranes under sub-critical conditions. However, it was also
postulated that increasing the pore size may decrease the depo-
sition onto the membrane at the expense of internal adsorption.
Long-term trials confirmed this theory as progressive internal
deposition eventually leads to catastrophic increase in resistance
[14,95]. This again emphasizes the importance of test duration
in fouling studies.
3.1.1.2. Porosity/roughness. Membrane roughness and poros-
ity were suggested as potential reasons for the different fouling
behaviors observed when four MF membranes with nominal
pore sizes narrowly ranged between 0.20 and 0.22 m were
tested in parallel [96]. The four membranes were operated under
the same constant pressure, and therefore produced different
initial fluxes. The track-etched membrane, with its dense struc-
ture and small but uniform cylindrical pores, featured the lowest
resistance due to pore fouling. In contrast, the other three mem-
branes presented interwoven sponge-like microstructures and
were more prone to pore fouling due to their highly porous net-
work. Although all membranes featured similar nominal pore
size, polyvinylidene fluoride (PVDF), mixed cellulose esters
(MCE) and polyethersulfone (PES) membranes presented dif-
ferent fouling behaviors. While fouling was mainly due to cake
formation for the PVDF and MCE membranes, pore block-
ing was responsible for 86% of the total hydraulic resistance
when the PES membrane was used. Overall, the PES membrane
showed a 50% higher fouling resistance than the PVDF and
MCE membranes. It was suspected that membrane microstruc-
ture, material and pore size distribution were all affecting MBR
fouling significantly [96]. Comparison between two microp-
orous membranes prepared by the stretching method revealed the
influence of the pore aspect ratio (mean major axis length/mean
minor axis length) on fouling in an MBR. With both membranes
the average pore size and pure water flux were identical, but less
fouling was observed with the membrane having the higher pore
aspect ratio (elliptical pore) rather than with the circular pore
membrane [97]. With roughness values (measured by AFM)
ranging from 2.4 to 33.2 nm, for 20 and 70 kDa MWCO mem-
branes, respectively, initial fouling was observed to decrease
while irreversible resistance increased [87]. However, in this
study based on an anaerobic MBR, membrane morphology and
pore size were changing simultaneously, so it was not possible
to clearly determine the effect of roughness on MBR fouling.
However, an assumption was made that the large filling-in
points present on rougher membranes are more prone to the
creation of fouling layers, compared to the fewer and smaller
crevices observed on smoother membranes [87]. Detailed dis-
cussion about the effect of membrane surface properties on cell
attachment could be found in [98], while Ho and Zydney gave
more details about membrane morphology and MBR fouling
[99].
3.1.1.3. Membrane conguration. The current trend in MBR
in the majority of the studies dealing with domestic wastewa-
ter treatment. As a result, comparison between these two MBR
configurations will be discussed only briefly in this review, but
more details can be found in [100103]. Based on short-term
critical flux tests, a direct comparison between submerged and
sidestream MBRs showed that similar fouling behavior was
obtained when the two configurations operated at superficial gas
velocity (UG ) of 0.070.11 m/s and superficial liquid velocity
(UL ) of 0.250.55 m/s for submerged and sidestream, respec-
tively [102]. An increase of UG in the submerged MBR was
also found to have more effect in fouling removal than a similar
raise of CFV (or UL ) in the sidestream configuration (also see
Section 3.3.1). This may be due to the benefit of unsteady state
flow achieved by bubbling.
In submerged MBR processes, the membrane can be con-
figured as vertical flat plates, vertical or horizontal hollow fine
fibers (filtration from out-to-in) or, more rarely as tubes (filtration
from in-to-out). Although the tubular configuration is generally
preferred for sidestream processes, the effect of the lumen size
on submerged MBR fouling has been investigated [104,105].
While hollow fiber modules are generally cheaper to manufac-
ture, allow high membrane density and can tolerate vigorous
backwashing, fluid dynamics and distributions may be probably
easier to control for flat plate and tubular membranes, where
the membrane channel width is well defined [106]. As a result,
hollow fibers may be more prone to fouling and require more
frequent washing and cleaning. An interesting discussion of the
relative performances of hollow fibers and flat plate membranes
was initiated by Gunder and Krauth [107] and revealed the bet-
ter hydraulic performance of the flat plate in their studies. Two
types of submerged MBR of comparable size, operated for the
same length of time for sewage treatment have also been com-
pared [108]. The differences observed were mostly due to the
different operating and maintenance conditions (see Section 4.1)
rather than the module designs per se. Although the price of the
flat plate MBR is estimated to be 2025% higher than hollow-
fiber-based-systems, fouling rate and maintenance operation are
generally less for the former configuration. This observation may
be due to the design flux at which MBR were operated in this
study, i.e. 2027 l/m2 h for flat plate and 2333 l/m2 h for hol-
low fiber [108]. The backwashing requirement of the hollow
fiber MBR (up to 25% of the permeate volume [108]) may also
slightly complicate the process. In another study, the effect of
membrane configuration was assessed when hollow fiber and
flat plate MBRs (featuring similar pore size of 0.4 m) were
used for high-strength wastewater treatment [109]. Once both
systems were operated at similar flux, it was found that the
flat sheet MBR fouled slightly more and could not recover its
original performance after water cleaning. However, chemical
cleaning managed to remove most of the fouling (probably due
to pore blocking in this specific case). Finally, each configu-
ration has specific footprint, airflow requirement, and integrity
testing which may favor one process over another one for a given
application. More details about these two configurations (with a
focus given on aeration intensity) and the effect of their physical
parameters are available from Cui et al. [106].
Amongst the numerous membrane manufacturers, Kubota
(flat plate configuration), Zenon, Mitsubishi and US Filter (hol-
low fiber configuration) are the main membrane suppliers for
MBR systems. Few large-scale studies based on comparison
of these commercially available MBR systems have been con-
ducted. The city of San Diego, California, and the research
consultant, Montgomery Watson Harza, have been evaluating
the MBR process through various projects since 1997, including
feasibility of using MBR to produce reclaimed water [110,111],
optimization of MBR operation, and parallel comparison and
cost estimations of the four leading MBR suppliers [112]. MBRs
were evaluated for their ability to produce high quality effluent
and to operate with minimum fouling. In terms of hydraulic
performances, it was shown that all four processes were able
to cope with flux rates exceeding 33 l/m2 h and HRTs as low
as 2 h. A 6-year-development programme has also been initi-
ated for the introduction of MBR technology in the Netherlands
market. Started in 2000, a comparative study of four 750 m3 /day-
MBRs carried out by DHV water has been reported [113,114].
Finally, three MBR plants, treating a design flow of 300 m3 /day
each, have been operated in parallel during 2003 and 2004 in
Singapore. This most recent study reported MBR power con-
sumption of less than 1 kWh/m3 of treated water [115], while
energy consumption around 1.9 kWh/m3 was reported for 2001
[116] and up to 2.5 kWh/m3 in 1999 [117]. Although these three
studies have been conducted with the MBR systems running in
parallel (with the same influent water), the MBR maximum flux,
operating conditions and general design applied were those rec-
ommended by the suppliers, and therefore somewhat different
for each system. This makes it difficult to make a fair compar-
ison, so it is not possible to classify the MBRs as a function of
their relative hydraulic performances, which need to be consid-
ered along with the cleaning protocols applied to each system
(see Section 4.1).
An important parameter for submerged hollow fibers is likely
to be packing density. The distance between adjacent membranes
is suspected to directly impact on mass transfer and therefore
the shear and aeration demands. Moreover, increasing the pack-
ing density could lead to severe clogging by gross solids and
to the slower rise of bubbles, limiting their effect on fouling
limitation. Experiments carried out with a model bundle of nine
fibers revealed the overall module performance to be much worse
than that of an individual fiber [118,119]. It was also clearly
shown that the surrounded fibers are less productive than the
outer fibers. At high feed concentration and low cross-velocity,
surrounded fibers become completely blocked and eventually
produce negligible flux. Finally, it was advised that the pack-
ing density should be lower than 30% in order for the bundle to
perform similarly to single fibers. In low packing density config-
urations, cake layers from adjacent fibers do not interfere with
each other and the effect of CFV may be more evenly distributed,
limiting overall fouling [119]. A mathematical model based on
substrate and biomass mass balance also revealed the significant
role played by packing density in the overall MBR performance,
and the hydrodynamics of the biomass in particular [120].
The effects of other membrane characteristics including hol-
low fiber orientation, size and flexibility are discussed in the
review of Cui et al. [106]. For hollow fiber membranes used
for yeast filtration, higher critical fluxes were measured for
slightly loose membranes (95%), with small diameter (0.65 mm)
and greater length (80 cm) [121]. Contradictory results showing
slightly higher specific flux for shorter membranes (30 cm cf.
100 cm) has been reported [122]. The pressure drop due to the
permeate flow in the lumen of the hollow fiber could be the main
cause behind the effect of membrane length on rapid and severe
fouling. Significant pressure loss (up to 53 kPa) was measured
for long fibers (60 cm). Below the critical length of 15 cm, pres-
sure loss was minimal at less than 11 kPa [97]. Further discussion
of fouling distribution in hollow fibers can be found elsewhere
[31,123127].
3.1.2. Chemical parameters
3.1.2.1. Hydrophobicity. Because of the hydrophobic interac-
tions occurring between solutes, microbial cells and membrane
material, membrane fouling is expected to be more severe with
hydrophobic rather than hydrophilic membranes [92,128130].
In many reported studies, change in membrane hydrophobic-
ity often occurs with other membrane modifications such as
pore size and morphology, which make the correlation between
membrane hydrophobicity and fouling more difficult to assess.
In a recent study for example, the contact angle measurement
showed that the apparent hydrophobicity of polyethersulfone
(PES) membranes decreased (from 55 to 47 ) with the increase
in MWCO (from 20 to 70 kDa membranes, respectively) [87].
The effect of membrane hydrophobicity was studied in detail
during comparison of two UF membranes of similar character-
istics [131]. Based on the greater solute rejection and fouling
and cake resistances reported for the hydrophobic membrane,
the authors were able to postulate on the effects of membrane
fouling on the removal performances of the MBR process. It
was concluded that the greater solute rejection was mainly due
to the dynamic layer formed by adsorption and/or sieving in the
cake deposited on the membrane, and, to a lesser extent, due to
direct adsorption into membrane pores and on the surface.
Numerous anti-fouling studies have been based on membrane
surface modification, and will be reviewed in Section 4.2.1.
Surprisingly, Fang and Shi [96] indicated that membranes of
greater hydrophilicity tend to be more vulnerable to deposition
of foulants of hydrophilic nature. In MBRs, activated sludge con-
tains substantial amounts of hydrophilic EPS, which has been
identified as an important foulant (Section 3.2.5). However, in
this study, the most hydrophilic membrane also featured more
open pores, which could be another reason for severe fouling.
Notwithstanding the significance of the membrane hydropho-
bicity on the early stage of the fouling formation, this parameter
is expected to play only a minor role during extended filtration
periods. Once initially fouled (i.e. conditioned), the membranes
chemical characteristics would become secondary to those of the
sludge materials covering the membrane surface.
3.1.2.2. Materials. Although featuring superior chemical, ther-
mal and hydraulic resistances, ceramic membranes are not the
preferred option for MBR applications due to their high cost.
However, ceramic membranes have been successfully used for
several MBR applications, such as treatment of high-strength
industrial waste [132,133] and anaerobic biodegradation [134].
Ceramic membranes, in modules which require higher pressure
and turbulence, are generally used in sidestream configura-
tions. The benefit of turbulence promoters in such MBR sys-
tems has been reported [135]. The potential advantage of using
ceramic membrane was demonstrated in a test comparing 0.1 m
ceramic with 0.03 m polymeric multi-channel membrane mod-
ules operated in sidestream air-lift mode. The ceramic MBR did
not substantially foul for short-term experiments with fluxes up
to 60 l/m2 h, while the polymeric membrane critically fouled at
around 36 l/m2 h [136]. However, in the same study, the over-
all cost of the ceramic membrane was reported to be around an
order of magnitude more expensive than the polymeric materials.
Finally, novel stainless steel membrane modules have recently
shown good hydraulic performance and fouling recovery when
used in an anaerobic MBR for wastewater treatment [137]. How-
ever, the large majority of the membranes used in MBRs are
polymeric-based. A direct comparison between polyethylene
(PE) and PVDF membranes clearly indicated that the later leads
to a better prevention of irreversible fouling and that PE mem-
brane fouled more quickly [138]. In that same study, the authors
also mentioned that the composition of the irreversible fouling
was dependant of the membrane material, as some fractions of
the organic matter present in the biomass presented a higher
affinity with certain polymeric materials.
3.2. Feedbiomass characteristics
3.2.1. Nature of feed and concentration
Although the effects of wastewater properties on mem-
brane fouling are undeniable for direct wastewater filtration
[139141], fouling in the MBR is mostly affected by the interac-
tions between the MBR membrane and the biological suspension
rather than wastewater per se [88]. However, in the rare cases of
using saline sewage as feed, the resulting higher fouling rate gen-
erally leads to a more frequent cleaning [142]. The most strik-
ing effect of the wastewater nature is on the physico-chemical
changes in the biological suspensions [13,14]. For example, the
protein fraction measured in the extracted EPS (eEPSp) has been
found to be significantly lower when biomass was fed with syn-
thetic feed (chemical oxygen demand: COD of 460 mg/l) rather
than with real sewage (COD of 140 mg/l). Simultaneously, the
fouling rate was higher using synthetically fed MBR [14]. For
these reasons, the fouling propensity of the wastewater is indi-
rectly taken into consideration during the characterization of the
biomass (Section 3.2.3).
3.2.2. Biomass fractionation
Activated sludge biomass can be fractionated into three ide-
alized components, i.e. suspended solids, colloids and solutes.
This approach has often been applied to account for the rela-
tive contribution of each biomass fraction on MBR fouling. The
methodology applied to appropriately separate the biomass frac-
tions varies from one study to another but remains a crucial step
in the definitions of the different biomass fractions and there-
fore, the interpretation of the results. Unfortunately, no standard
method exists. However, Fig. 7 shows a typical protocol where
the biomass sample is centrifuged, the resulting supernatant is
then filtered with a dead-end membrane cell, with the calculated
hydraulic resistance (Rsup ) being attributed to colloidal and sol-
uble species (Rcol and Rsol , respectively). Another portion of
the biomass suspension is then filtered by a microfilter (with
nominal pore size of around 0.5 m). The fouling properties of
this coarse-filtered supernatant are attributed solely to the solu-
ble matter with resistance Rsol . Calculations assess the relative
fouling contributions of the suspended solids and the colloids
[143]. In another approach, the concentration of colloids was
also characterized by the difference between the levels of TOC
present in the filtrate passing through 1.5 m filtration paper and
in the permeate collected from the MBR membrane (0.04 m
membrane) [29]. Although fractionation methods may signif-
icantly vary for different studies (see references from Fig. 8),
results are often reported in terms of hydraulic resistances for
suspended solids (Rss ), colloids (Rcol ) and soluble species (Rsol ),
the sum of which being the total resistance (Rt ).
Although an interesting approach for studying MBR fouling,
the fractionation experiment neglects any coupling or synergistic
effects which may occur among the different components of the
biomass. The interactions between each biomass fraction and the
operating conditions are numerous and include the type of feed
water used [144], permeability of the membrane, particle size
and hydrodynamics conditions [143]. Examples of interactions
between suspended and dissolved solids and membrane fouling
Fig. 7. Experimental method for the determination of the relative fouling
propensity for the three biomass fractions.
 seems to decrease fouling at low MLSS concentration (<6 g/l),
more fouling is expected as the MLSS concentration increases
above 15 g/l. The level of MLSS does not appear to have signif-
icant effect on membrane fouling between 8 and 12 g/l. Another
study [153] reviewed the significant effect of MLSS for con-
centrations lower than 5 g/l, and indicated that hydrodynamics
(more than MLSS concentration) control the critical flux (Jc )
for greater MLSS levels [153]. This is only partially verified
by the data reported in Table 3. More subtle studies showed
apparent contradictory trends from data obtained in the same
study. For example, the cake resistance (Rc ) was observed to
increase and the specific cake resistance (c ) to decrease as
MLSS increased. Although having similar meaning conceptu-
ally Rc and c seemed to behave inversely [146]. This can be
Fig. 8. Relative contributions (in %) of the different biomass fractions to MBR reconciled by noting:
fouling. For SRT increase from 8 days (1) to 40 days (2); F/M ratio of 0.5, results
based on modified fouling index (3); based on flux reduction after 600 min of Rc = c mc (1)
each fraction filtration (4); for SRT increase from 20 days (5) to 60 days (6).
where mc is the cake load/area of membrane. The cake load mc
would tend to rise with MLSS concentration. Bin et al. observed
were discussed in Section 2.3. The protocol illustrated in Fig. 7
the permeate flux to decrease (but at a lower fouling rate) when
is limited because it relies on dead-end filtration tests with a
MLSS increased [154]. This was explained by the creation of a
specific membrane. However, studies on biomass fractionation
rapid fouling cake layer (potentially protecting the membrane) at
have also been reported for crossflow and submerged configu-
high concentration, while progressive pore blocking created by
rations. An attempt to compare results obtained from different
colloids and particles was thought to take place at lower MLSS
studies is reported in Fig. 8 where relative contributions have
concentration.
been calculated.
Since the value of Jc is often determined during short-term
The relative contribution of the biomass supernatant (soluble
experiments, it is expected that Jc indicates the deposition of
and colloids, generally defined as soluble microbial products
suspended solids rather than colloidal and soluble materials. As a
or SMP) to overall membrane fouling ranges from 17% [143]
result, the flux value at which the experiment is carried out, has a
to 81% [145]. These wide discrepancies may surprise and are
significant impact on the determination of the effect of the MLSS
probably explained by the different operating conditions and
concentration. Similarly, the test duration can be a factor. While
biological states of the suspension used in the reported stud-
MBR performances are expected to decrease for higher MLSS
ies. They also confirmed the relatively low fouling role played
(at applied flux superior to Jc ), the MLSS concentration may not
by the suspended solids (biofloc and the attached EPS) com-
pared to those of the SMP (Section 3.2.6). In terms of fouling
mechanisms, soluble and colloidal materials are assumed to be Table 3
Influence of shift in MLSS concentration (g/l) on MBR fouling
responsible for the pore blockage of the membrane, while sus-
pended solids account mainly for the cake layer resistance [145] MLSS shift Fouling parameters References
(Section 3.4.2). However, because MBRs are typically operated Fouling increase
at modest flux, the formation of a biomass cake tends not to 0.093.7 Rc : 21 to 54 1011 m1 and c : 18.5 to [146]
occur. The smaller species (like SMP) are much more likely to 0.7 108 m/kg
deposit. 2.49.6 Rp : 9 to 22 1011 m1 [96]
718 Jc : 4736 l/m2 h (for SRT: 30100 days) [155]
2.19.6 Jc : 138 l/m2 h [154]
3.2.3. Biomass (bulk) parameters 110 Jc : 7535 l/m2 h [92]a
3.2.3.1. MLSS concentration. Often considered at first sight as 215 Limiting flux: 10550 l/m2 h [156]a
the main foulant parameter, MLSS concentration has indeed a 1.622 Stabilized flux: 6525 l/m2 h [157]a
complex interaction with MBR fouling, and controversial find- Fouling decrease
ings about the effect of this parameter on membrane filtration 3.510 Jc : <60 to >80 l/m2 h [26]a
have been reported. If the other biomass characteristics are not No (or little) effect
accounted for, the increase in MLSS concentration seems to have 914 No impact on fouling rate [158]
a mostly negative impact (higher TMP or lower flux) on the MBR 4.411.6 No impact between 4 and 8 g/l, slightly [84]
less fouling for 12 g/l
hydraulic performances [146,147]. However, some authors have 618 Similar fouling rates for J < 10 l/m2 h, [148]
reported positive impact [26,148], and some observed insignif- and slightly lower fouling rates for
icant impact [84,149,150]. The existence of a threshold above higher J
which the MLSS concentration has a negative influence was also 415.1 Jc decreased from 25 to 22 l/m2 h [24]
reported (at 30 g/l [151]). A more detailed fouling trend has been 3.68.4 [149]
a
described by Rosenberger et al. [152]. While a rise in MLSS Sidestream MBR.
play a significant role in fouling propensity when the MBR is
operated at low fluxes. In that later case, EPS components and
concentrations have more effect on the MBR fouling than the
MLSS concentration (Sections 3.2.5 and 3.2.6). Contradictory
results may also arise from the mode of filtration, i.e. constant
flux versus constant TMP (Section 3.4).
Empirically derived equations predicting flux performance
have been proposed in numerous papers [96,159161]. How-
ever, these equations have limited use as they are generally
obtained under very specific conditions and take into account
some specific operating parameters and disregard some others.
A mathematical expression linking MLSS concentration, EPS
and TMP with cake specific resistance has been proposed by
Cho et al. [162]. In this study, specific resistance did not change Fig. 9. Viscosity obtained at different MLSS concentrations and shear rates
significantly for MLSS ranging from 4 to 10 g/l and when the [105].
EPS and TMP were kept constant.
The experimental method used for changing MLSS con- plastic (or shear-thinning) property of the sludge obtained in
centration can also significantly impact upon biomass charac- MBR.
teristics since biomass acclimatization periods are not always
respected [147]. Although the removal performances are gener-
3.2.3.3. Temperature. Temperature impacts on membrane fil-
ally high for MBR processes, MLSS concentration also plays a
tration through its influence on the permeate fluid viscosity
significant role in this regard. For example, an optimal MLSS
[168]. The common approach to comparing hydraulic perfor-
concentration at 6 g/l was obtained based on the highest COD
mance obtained at different temperatures is to normalize the
removal [163] and on the highest virus removal [164].
operating flux at a reference temperature (generally 25 C). This
The lack of a clear correlation between MLSS concentration
could be done by applying a temperature correction factor [169].
and any other foulant characteristics indicates that the MLSS
To avoid the interference of the temperature effects on MBR
concentration (alone) is a poor indicator of biomass fouling
fouling, non-linear regression between critical flux and temper-
propensity [13,165]. These authors recommended the use of fun-
ature was obtained [29]:
damental operating parameters like HRT and SRT for prediction
of foulant production. This has been supported by the relatively Jc,t = Jc,20 1.025t20 (2)
stable foulant characteristics obtained once true steady-state was
established in the bioreactor. Current studies tend to consider Interestingly, experiments carried out at two sets of temper-
the non-settleable organic substances (rather than the MLSS atures (1718 and 1314 C) featured different hydraulic resis-
concentration) as the main players in the fouling propensity in tances even after the flux had been normalized [170]. The greater
MBRs (see Sections 3.2.5 and 3.2.6). resistances observed at low temperature were explained by four
phenomena occurring in the system: (1) within that temperature
3.2.3.2. Viscosity. In the MBR, like in conventional activated range, the sludge viscosity (rather than permeate viscosity) was
sludge processes, biomass viscosity is closely related to its con- calculated to increase by 10%, reducing the shear stress gener-
centration, and has been cited as a foulant parameter [166]. ated by coarse bubbles, (2) intensified defloculation tend to occur
A critical MLSS concentration exists under which the viscos- at low temperature, reducing biomass floc size and releasing
ity remains low and rises only slowly with the concentration. EPS to the solution, (3) particle back transport velocity, calcu-
Above this critical value, suspension viscosity tends to increase lated with the Brownian diffusion coefficient (linearly related to
exponentially with the solids concentration [145]. This criti- temperature), is less at low temperature, and (4) biodegradation
cal value was observed to change from 10 to 17 g MLSS/l for of COD was also reduced at decreased temperature, resulting in
different operating conditions (conventional and hybrid (pre- a higher concentration of solute and particle COD in the reactor
coagulation/sedimentation) MBRs, respectively). Similar obser- [170]. This last phenomenon was also observed by Fawehinmi
vations were reported for the behavior of the capillary suction et al. [171] with higher SMP levels measured in an anaerobic
time (CST), another parameter closely related to viscosity [30]. MBR operated at 20 C rather than at 30 C. All of these fac-
The importance of MLSS viscosity is that it modifies bubble tors are directly linked to membrane fouling, so it is expected to
size and can dampen the movement of hollow fibers in sub- observe greater deposition of materials on the membrane surface
merged bundles [121]. The net result of this phenomenon would at lower temperatures [158].
be a greater rate of fouling. Increased viscosity also reduces
the efficiency of mass transfer of oxygen and can therefore 3.2.3.4. Dissolved oxygen (DO). The average level of DO in
effect dissolved oxygen (DO) [167]; fouling tends to be worse the bioreactor is controlled by the aeration rate, which not only
at low DO (see below). The effect of MLSS concentration on provides oxygen to the biomass but also tend to limit foul-
viscosity at different shear rates obtained from a submerged ing formation on the membrane surface. The effects of DO on
MBR is shown in Fig. 9. These results also indicate the pseudo- MBR fouling are therefore multiple and may include changes in
biofilm structure, SMP levels, and floc size distribution [89]. As
a general trend, higher DO tends to lead to better filterability, and
lower fouling rate. This was explained by the lower specific cake
resistance of the fouling layer which featured larger particle sizes
and greater porosity [172,173]. As expected, significant differ-
ences were observed in microbial communities and resulting
biofouling when the MBR was operated under various DO lev-
els (from 6 to less than 0.1 mg/l in [172]). Surprisingly, the COD
in biomass suspension (i.e. an indicator for SMP level) decreased
from 37 to 27 mg/l for DO of 3.4 and 0.9 mgO2 /l, respectively
[174] and therefore cannot explained the hydraulic performances
obtained in MBR operated at higher DO. Moreover, the con-
tribution of SMP to membrane filterability was found to be a
minimum compared to those of the physico-chemical proper-
ties of cake layer (i.e. particle size and porosity) [173]. In a
study obtained with anoxic and aerobic sludges [175], floc dete-
rioration was observed and used as a possible explanation for
the higher fouling rates obtained for the denitrification assay.
The effect of oxygen limitation causing a lowering of the cell
surface hydrophobicity, and consecutive floc deterioration, was
concluded to be the main reason for the worsen MBR fouling
for anoxic conditions.
In the MBR, fouling may also be due to the creation of a
biofilm layer on the membrane surface. As a general definition,
bacterial biofilm characterizes the population of microorgan-
isms concentrating, depositing and/or growing at the solid/liquid
interface [176]. As described later in the review (Section 3.2.5),
the formation of biofilms is possible through the active role
of EPS which surround the microorganisms. Biofilm proper-
ties such as adhesion strength (interaction between microorgan-
isms and membrane) and cohesion strength (interaction between
microorganisms themselves) can be determined and are directly
dependant of the nature of the EPS [176]. As the thickness of
the biological fouling layer increases with extended MBR filtra-
tion time, some biofilm regions have been observed to become
anaerobic [86]. Because of the poor oxygen transfer within the
biofilm structure, the fouling sub-layers (on the membrane sur-
face) may become anaerobic, and therefore affect membrane
fouling differently. Endogenous decay, similar to that expected
within the fouling layer, was simulated and revealed the level
of carbohydrate in the extracted EPS (eEPSc) to significantly
increase. Since the transition between aerobic to anaerobic con-
ditions seems to produce a large amount of EPS, this phe-
nomenon could also be responsible for MBR fouling [86].
More details about fouling in anaerobic MBR can be found
in [1].
The direct impact of air bubbles (as a foulant parameter) on
MBR filtration was even investigated by Jang et al. However, it
was concluded that the effect of air blocking on the surface can
be ignored in MBR processes with high MLSS concentration
(as it accounted for less than 1% of total resistance Rt ) [177].
However, under some circumstances, air bubbles my be present
or be formed in the lumens of hollow fibers and this can be
detrimental [178]. Finally, it is important to keep in mind that
the aeration rate (discussed in Section 3.3.1) controls biological
requirements and parameters such as DO, ammonium/nitrate
ratio [179].
3.2.4. Floc characteristics
3.2.4.1. Floc size. In MBR systems, aggregation of the
microorganisms, and the formation of large floc is a signifi-
cant element in the effective separation of suspended biomass
from the treated water, although it is more critical in CASP.
In terms of floc size, biomass suspensions in MBRs feature a
wide distribution, which ranges significantly from one study to
another. Comparison of the aggregate size distribution of CASP
and MBR sludges was carried out [180] and revealed a distinct
difference in terms of mean particle sizes (160 and 240 m,
respectively). A bimodal distribution was even observed for
MBR sludge (520 and 240 m); the high concentration of small
colloids, particles and free bacteria was caused by their com-
plete retention by the membrane. In this study, sludges were
collected from small-scale experimental rigs and measured by
particle size analyzer (MasterSizer 2000). In another study, par-
tial characterization of the floc (up to 100 m) reported the floc
size to range from 10 to 40 m, with a mean size of 25 m
[143]. These authors also claimed that the floc size distribution
obtained with the MBR sludge are lower than the results gener-
ally obtained from CASP. In comparison, the particles present
in the supernatant, obtained after 4 h of gravitational sedimenta-
tion, have a mean size of around 9 m. The floc size distributions
obtained with three MBR operated at different SRTs were sim-
ilar, although the mean floc size increased slightly from 5.2 to
6.6 m for SRT increasing from 20 to 60 days [181].
Given the large size of the floc particles, compared to the pore
size of the membrane generally used in MBR, it is expected
that floc cannot directly block pore entrances. Nor would the
floc deposit on the membrane surface due to drag forces result-
ing from the low/modest fluxes and the shear induced back
transport phenomenon experienced by large particles. However,
independent of their size, biological floc play a major role in
the formation of the fouling cake on the membrane surface. The
effect of the EPS level on floc size will be discussed in Sec-
tion 3.2.5. The addition of aerobic granules, activated carbon or
polymer can significantly increase the floc size. Their effect on
MBR fouling is reported in Section 4.2.2.
3.2.4.2. Hydrophobicity/surface charge. In the MBR process,
like in CASPs, hydrophobic flocs lead to high flocculation
propensity and low interaction with the (generally) hydrophilic
membrane. However, reports of highly hydrophobic flocs foul-
ing MBR membranes can be found in the literature. Relative
hydrophobicity of floc can be directly measured by bacterial
adhesion to hydrocarbons (hexane) [182], or estimated by con-
tact angle determination [128]. Although the direct effect of floc
hydrophobicity on MBR fouling is difficult to assess, hydropho-
bicity measurement of sludge and EPS solutions revealed that
the decrease of EPS relative hydrophobicity may cause floc dete-
rioration (and consequent increase of Rc ) [175,182]. EPS level
and filamentous index (parameter related to the relative pres-
ence of filamentous bacteria in sludge) have a direct influence
on the relative hydrophobicity and zeta potential measured in
the biomass floc. The excess growth of filamentous bacteria,
known to be responsible for severe MBR fouling, also resulted in
higher EPS levels, lower zeta potential, more irregular floc shape

Fig. 10. Simplified representation of EPS, eEPS and SMP.
and higher hydrophobicity [183]. In another example, foam-
ing sludge showed greater flux decline (more than 100 times)
than the non-foaming sludge. The increase was attributed to the
hydrophobic and waxy nature of the foaming sludge surface
[184].
Due to the negative charges from ionization of the anionic
functional groups, flocs (and EPS) of most activated sludge fea-
ture zeta potential and surface charges ranging from 0.2 to
0.6 mequiv./g VSS and from 20 to 30 mV, respectively
[185]. The surface charge of MBR microbial floc (obtained by
the titration method) confirms the general trend, as it ranged
from 0.7 to 0.4 mequiv./g VSS when the MBR was operated
at various SRT (from 20 to 60 days) [181]. This was accompa-
nied by an increase in contact angle (from 34 to 44 ). In this
study where the fouling resistance caused by microbial floc was
found to increase with the SRT, contact angle and surface charge
demonstrated a strong positive correlation with the microbial-
floc-caused fouling propensity. For CASP, Liu and Fang also
reviewed a positive effect of long SRT on hydrophobicity and
flocculation [185].
3.2.5. Extracellular polymeric substances (EPS)
Given the large number of recent publications dealing with
the fouling of MBRs by bio-polymeric substances, a major
section of this review is focused on their nature, method of deter-
mination and influence on MBR fouling.
Extracellular polymeric substances (EPS) are the construc-
tion materials for microbial aggregates such as biofilms, flocs
and activated sludge liquors. The term EPS is used as a gen-
eral and comprehensive concept for different classes of macro-
molecules such as polysaccharides, proteins, nucleic acids,
(phosphor-)lipids and other polymeric compounds which have
been found at or outside the cell surface and in the intercellular
space of microbial aggregates [186]. They consist of insoluble
materials (sheaths, capsular polymers, condensed gel, loosely
Fig. 11. Proposed method for EPS and SMP extractions and measurements.
bound polymers and attached organic material) produced by
active secretion, shedding of cell surface material or cell lysis
[175]. The functions of EPS matrix are multiple and include
aggregation of bacterial cells in flocs and biofilms, formation
of a protective barrier around the bacteria, retention of water
and adhesion to surfaces [187]. With its heterogeneous and
changing nature, EPS can form a highly hydrated gel matrix
in which microbial cells are embedded [188]. Therefore they
can be responsible for the creation of a significant barrier to per-
meate flow in membrane processes. Finally, bioflocs attached
to the membrane can play a major nutrient source during the
biofilm formation on the membrane surface [189]. Their effects
on MBR filtration have been reported for more than a decade
[190] and have received considerable attention in recent years
with many reports indicating the EPS to be the most significant
factor affecting fouling in MBRs [83]. In this review, distinc-
tion will be made between the EPS extracted artificially from
the biological cell floc (eEPS) and the soluble EPS present in
the activated sludge supernatant and unassociated with the cell
(soluble microbial products or SMP). The term EPS is used
as a general parameter to characterize bio-polymeric substances
in the reactor (Fig. 10). It is important to recognize that the
exact definitions of eEPS, and SMP are directly dependant of
the methods used to obtain and characterize chemically these
solutions.
Studies on the effects of EPS in MBR fouling rely on extrac-
tion of EPS from the sludge floc. So far, no standard method of
extraction exists, making comparison between research groups
difficult. Methods of extraction are numerous and include cation
exchange resin [175,191,192], heating methods [193], centrifu-
gation with formaldehyde [194]. These techniques, along with
others, have been compared under various conditions to assess
their efficacies [185], and results have revealed that formalde-
hyde extraction was the most effective to extract the largest
concentration of eEPS. However, because of its simplicity, the
heating method is sometimes preferred (Fig. 11). Typically, the
solution containing eEPS is then characterized by its relative
content of protein (eEPSp) and carbohydrate (eEPSc), measured
by photometric methods (Lowry et al. [195] and Dubois et al.
[196] methods, respectively). Although the EPS characterization
is sometimes reported in terms of polysaccharides, this review
will only use the term carbohydrate, which definition comprises
compounds like polysaccharides. While eEPSp has generally a
hydrophobic tendency, eEPSc is more hydrophilic [185]. eEPS
Table 4
Concentration of the eEPS components in different MBR systems (units are in mg/gSS by default)
eEPSp eEPSc Other Details References

2530 78 Humic: 1213 R (10) [180]

29 36 SUVA: 2.83.1 l/m mg S [199]a
120 40 S () [200]
31116 615 TOC: 3765 Four pilot-scale plants, municipal [165]
20 14 Pilot-scale plant, Industrial
1146 1240 TOC: 4447 Three full-scale plants, municipal
25 9 TOC: 42 Full-scale plants, industrial
EPSp + EPSc = 8 [175]
3036 3328 From 20 to 60 [181]
73 30 S () [14]
60 17 R ()
TOC: 250 mg/l S, MLSS: 14 g/l [198]
TOC: 2683 mg/gVSS From 8 to 80 [197]
116101 2224 S (20) [174]

S, synthetic wastewater; R, real wastewater; SRT are given in days in bracket; , infinite SRT (i.e. no wastage).
a Anaerobic upflow-sludge bed filter (UBF) and an aerobic MBR [199].

solution can also be characterized in terms of its TOC level ing) of the apparent molecular weight distributions of natu-
[197,198] and, less frequently, its aromaticity or hydrophobic- ral organic matters (NOM) [204]. The same technology was
ity (by the measurement of the specific ultraviolet absorbance applied to compare eEPS solutions obtained from different con-
(SUVA) [199]). Table 4 reports eEPS concentrations from var- figurations, operating conditions or treatment plants (Fig. 12).
ious MBR set-ups and reveals a relatively narrow range of the Preliminary results revealed, for example, the similarity of the
eEPSp and eEPSc levels measured. In most cases, eEPSp (with a eEPS profiles between different treatment plants [13,30,165].
maximum concentration of 120 mg/gSS) was greater than eEPSc This confirms previous findings obtained with CASP sludge.
(maximum concentration of 40 mg/gSS). Sludge flocs have also Size exclusion chromatography combined with infrared micro-
been characterized in terms of protein and carbohydrate levels, spectroscopy techniques was used for CASP sludge [191].
with colorimetric analysis carried out directly from the washed
biomass [174]. Low correlation was found between these two
new indicators and MBR fouling propensity. Finally, the mea-
surement of humic substances, generally overlooked for protein
and carbohydrate, have revealed their significant occurrence in
activated liquors [185], and may require more attention in future
research on MBR fouling.
As mentioned before, EPS has been identified as a major foul-
ing parameter [25,184,201203]. More recently, a functional
relationship between specific resistance, MLVSS, TMP, perme-
ate viscosity and eEPS was obtained by dimensional analysis
[197]. eEPS was found to have no effect on the specific resistance
below 20 and above 80 mgEPS/gMLVSS, but played a signifi-
cant role on MBR fouling between these two limits. This was
confirmed by another study reporting no clear relation between
bound EPS (or eEPS) and membrane fouling for concentrations
lower than 10 mg/gSS [138]. In another example obtained with
an anaerobic MBR, specific resistance increased linearly with
eEPS rising from 20 to 130 mg/gSS [171].
In order to reach a better understanding of membrane fouling
caused by EPS, further insights into eEPS identification were
recently obtained for MBR sludge [175,182]. In a study based
on an intermittently aerated MBR, eEPS solution featured three
main MW peaks at 100, 500 and 2000 kDa (fractionation con-
ducted by gel chromatography). In this example, eEPS with
MW larger than 1000 kDa was assumed to be mainly respon-
sible for MBR fouling [198]. For drinking water treatment,
high performance size exclusion chromatography (HPSEC) has Fig. 12. HPSEC profiles of eEPS (a) and SMP (b) from municipal plants oper-
been widely used for accurate characterization (or fingerprint- ated at different MLSS concentrations [13].
Resulting chromatographs of eEPS solution exhibited seven
distinct peaks. The analysis of the complex mixtures of eEPS
polymers revealed the presence of 45670 kDa MW proteins,
and 0.51 kDa MW carbohydrates. The presence of both pro-
teins and carbohydrates around the biological cells was proposed
as a key parameter in the floc formation, and therefore may also
have a significant role in MBR fouling. From this point of view,
the work reported for characterization of eEPS obtained from
CASP and their influence of flocculation, settling and dewater-
ing may also be an interesting parallel for MBR fouling. Recent
reviews [185,205] reporting these issues are valuable tools for
future EPSMBR studies.
Since the EPS matrix plays a major role in the hydrophobic
interactions among microbial cells and thus in the floc forma-
tion [185], it was proposed that a decrease in EPS levels may
cause floc deterioration. Experimental results obtained during
the comparative study of nitrification/denitrification in a MBR
tend to confirm this theory [175]. The repercussion of low EPS
level, and therefore floc deterioration on membrane fouling may
be detrimental for the MBR performances. If verified more thor-
oughly, this would indicate the existence of an optimum EPS
level for which floc structure is maintained without featuring
high fouling propensity.
Many parameters including gas sparging, substrate composi-
tion [171], loading rate [206,207] affect EPS characteristics in
the MBR, but SRT probably remains the most significant of them
[208]. A clear decrease of EPS levels was observed for extended
SRT, but this reduction became negligible for SRT greater than
30 days [165]. However, Lee et al. [181] observed an increase
in protein concentration (along with stable carbohydrate levels)
when SRT was increased. Further comments on the role of SRT
are given in Section 3.3.2.
3.2.6. Soluble microbial products (SMP)
In an attempt to protect the membrane from direct contact
with MLSS, a dual compartment MBR (bioreactor coupled with
settling tank in which membrane filters biomass supernatant)
has been built in Singapore [207]. In this set-up, higher fil-
tration resistance was observed from the membranes filtering
Table 5
Concentration of the SMP components (in mg/l)
SMPp SMPc Other
8 25 Humic subs: 36
314
26.5
TOC: up to 8 mg/l
0.59a n.d.10a 437a (TOC)
0.51a n.d. 11a
0.5a n.d. 1.5a
TOC: 3070 mg/l
23 7 R (not available)
DOC: 5 mg/l
TOC: 810 mg/l
1034 533
4.56 4.53.7
n.d., non-detected; S, synthetic wastewater; R, real wastewater; SRT are given in days in bracket; , infinite SRT (i.e. no wastage).
a In mg/gSS.
supernatant rather than those filtering 4 g/l of biomass. This
example clearly indicates that the composition and concentration
of the organics present in the biomass supernatant (i.e. soluble
microbial products (SMP)) have a large impact on membrane
performance. SMP are defined as soluble cellular components
that are released during cell lysis, diffuse through the cell mem-
brane, are lost during synthesis or are excreted for some purpose
[187,209]. In MBR systems, they can also be provided from the
feed substrate (Fig. 10). It has been now widely accepted that the
concepts of soluble EPS and SMP are identical [152,175,187].
During filtration, SMP adsorb on the membrane surface, block
membrane pores and/or form a gel structure on the membrane
surface where they provide a possible nutrient source for biofilm
formation and a hydraulic resistance to permeate flow [152].
Although the influence of dissolved matter has been studied for
a decade, the concept of SMP fouling in the MBR is relatively
new as no report on SMP levels existed for MBRs prior to 2001
[83]. In order to reveal the feasibility and relevance of liquid
phase analyses on MBR filterability and potentially standardize
the method, Rosenberger et al. reported four MBR cases studies
based on SMP analysis for membrane fouling [152].
Three methods of separating the water phase from the
biomass have been investigated, and the simple filtration through
filter paper was found to be the most effective technique over
centrifugation and sedimentation [210]. Although these authors
used a large pore filter paper (12 m), it is suggested in this
review to filter the solution with, at least, a 1.2 m filter in order
to remove colloids (Fig. 11). Similarly to eEPS, SMP solution
is then characterized with its relative amount of protein and
carbohydrate [210], with its TOC level [200] or more rarely
with SUVA measurement [211]. Examples of SMPp and SMPc
reported in the literature are given in Table 5.
HPSEC analysis has also been conducted on SMP solutions
(Fig. 12). Not surprisingly, the molecular weight distribution
of the organics present in MBR supernatant was found to be
significantly different for reactors operated under various con-
ditions [158]. However, the SMP solution fingerprint was largely
unchanged for weekly measurement from the same reactor, indi-
cating no significant change in SMP characteristics when the
Operating conditions References
R (10) [180]
R (8) [158]
R (15)
S () [200]
Four pilot-scale plants, municipal
Three full-scale plants, municipal [165]
Full-scale plant, industrial
S (), MLSS 15 g/l [212]
[210]
S (20) [211]
R (21) [115]
R (from 40 to 8) [213]
S (20) [174]
biomass is acclimatized to given operating conditions. When
compared to EPS molecular weight distribution, the SMP solu-
tion featured generally larger macromolecules [165].
Comparison between acclimatized sludges obtained from
MBR and CASP pilot plants revealed similar levels in terms
of eEPSp, eEPSc and eEPShumic [180]. The presence of the
membrane in the MBR process does not seem to affect the
content of eEPS within the flocs. However, SMPp, SMPc and
SMPhumic levels were significantly greater for the MBR sludge,
presumably due to the retention of large macromolecules by the
membrane. Critical flux tests carried out under the same condi-
tions for both MBR and CASP sludges revealed the higher foul-
ing propensity of MBR sludge over CASP (critical fluxes were
around 1015 and 3243 l/m2 h, respectively). Since the mea-
sured levels of EPS was unchanged, only the SMP components
can be accounted for the higher membrane fouling observed for
MBR sludge [180]. During this study, Cabassud and co-workers
observed significant biological activity in the MBR supernatant,
indicating the presence of free bacteria (presumably submicron
colloidal size), which could also be another cause of mem-
brane fouling. Direct linear relationships between loss of MBR
hydraulic performances and SMP concentration has been also
reported for an anaerobic MBR [171] and has been mathemat-
ically modeled [214]. Different mechanisms for the interaction
between the macromolecules present in the supernatant and the
membrane surface have also been proposed recently [158]. The
creation of the fouling layer on the membrane surface would
act as a secondary membrane, increasing the retention and/or
the adsorption of macromolecules. The formation of a biofilm
could also lead to the degradation of the macromolecules as
the permeate flows through the membrane. Finally, interaction
between the macromolecules and other solutes (humics, divalent
cations) within the membrane pores may be responsible for the
reduction of the membrane pore size over time.
In an attempt to define the biomass fraction with the highest
fouling potential, Lesjean et al. [150] conducted a methodi-
cal comparison between permeate and supernatant solutions.
Assuming that the materials observed in the biological super-
natant and not in the permeate solution are responsible for MBR
fouling, this group clearly revealed the higher concentration of
carbohydrates, proteins and organic colloids in the MBR super-
natant compared to those in the permeate. These findings con-
firmed similar results previously reported [30,210]. Since, direct
relationships between the carbohydrate level in SMP solution
with fouling rate [150], filtration index and CST [213,215,216],
critical flux tests [102], and specific flux [152] have been clearly
described, this reveals the SMPc as the major foulant indicator
in MBR systems. However, the nature and fouling propensity
of SMPc were observed to change during the study of unsteady
MBR operation [217]. In this specific study, it was not possi-
ble to correlate SMPc to fouling. So far, the effect of the protein
fraction contained in the SMP solution on MBR fouling has been
more rarely reported. Since a significant amount of proteins is
retained by the membrane (from 15% [210] to 90% [217]), it
is expected that this plays a role in MBR fouling. This was
recently confirmed by the value of specific resistance increasing
by a factor of 10 as the SMPp increased from 30 to 100 mg/l
[208]. However, in two separate studies, analyses of the foul-
ing layer have revealed a higher concentration of carbohydrate
and lower concentration of proteins compared to their levels in
the activated sludge [86,218]. This further confirms the greater
distribution of SMPc in the fouling layer compared to that of
SMPp. With a smaller MW, humic substances contained in the
liquid phase are not retained by the membrane, and therefore
may not significantly participate to MBR fouling [217].
As expected, many operating parameters affect SMP levels
in MBRs. As for eEPS, SMP levels decreased with increasing
SRT [165]. For SRT ranging from 4 to 22 days, SMPp and SMPc
levels were reduced by factors of 3 and 6, respectively [213]. In
their long-term study, Rosenberger et al. identified temperature
and stress to the microorganisms (and at a lower degree, SRT)
to be the main parameters affecting SMPc [158].
In order to obtain better control of the environmental con-
ditions, many research studies are based on the use of syn-
thetic/analogue solutions, which attempt to model real wastew-
aters. These solutions are sometimes very basic (mainly com-
posed of glucose) and therefore are very easily biodegradable.
As a result, it is expected that SMP levels in such systems are
lower than in real systems. Since it may be assumed that there are
almost no substrate residuals from glucose in the supernatant,
the less biodegradable SMP induced by cell lysis or cell release
would account for most of the SMP measured in synthetically fed
MBRs. This could explain the lower influence of SMP compared
to those of eEPS reported in some MBR studies. When using syn-
thetic substrate, Cho et al. [197] concluded that the membrane
fouling was affected more by the bound EPS of activated sludge
floc rather than the dissolved organic matter. SUVA measure-
ment carried out from supernatant of MBR fed with synthetic
solution confirmed the presence of a portion of larger, more aro-
matic, more hydrophobic and double-bond-rich organics, which
originated from the decayed biomass rather than the feed [211].
Another important study [219], also based on synthetic wastew-
ater, revealed that soluble organics alone cannot predict MBR
fouling. By comparing filterabilities of attached and suspended
growth microorganisms, Lee and co-workers observed the rate
of membrane fouling of the attached growth system (MLSS
0.1 g/l and attached biomass of 2 g/l) to be about seven times
higher than that of suspended growth MBR (MLSS of 3 g/l).
With similar soluble fraction characteristics in both reactors,
the filtration discrepancy was explained by the formation of a
protective dynamic membrane created by suspended solids. The
results of Ng et al. [207] reported earlier, with more fouling
from supernatant that mixed liquor, can also be explained by this
mechanism.
Another group of organic materials has been recently
introduced by Wang et al. [220]. The biopolymer clusters
(BPC) have been defined as non-filterable material issued from
the affinity clustering of the free EPS and SMP present in the
sludge cake deposited on the membrane surface. Although
BPC is expected to accumulate on the pore of the sludge cake,
this material can be readily separated from the fouling cake by
simple stirring. This work highlights the recent interest in the
polymeric characterization of the fouling layer [172,221]. For
this purpose, confocal laser scanning microscopy can be used
to precisely locate different EPS compounds on the membrane
surface [172,176,222,223].
3.3. Operating conditions
3.3.1. Aeration, crossow velocity
Controlling fouling in submerged membrane systems
remains more challenging than in pumped crossflow or dead-end
rigs, in which the feed-liquid can be more accurately managed.
Since the origin of the submerged MBR, bubbling has been
defined as the strategy of choice to induce flow circulation and
shear stress on the membrane surface. Aeration used in MBR
systems has three major roles: providing oxygen to the biomass,
maintaining the activated sludge in suspension and mitigating
fouling by constant scouring of the membrane surface [224]. The
use of gas bubbling to enhance membrane processes, and MBRs
in particular, has been thoroughly investigated and reviewed
[106]. While fundamental studies and mathematical models have
been applied to well-defined membrane configurations (such as
tubular [225,226] and flat sheet [227229]), the effect of bub-
bles on submerged hollow fiber modules is still being assessed.
More recently, the uneven distribution of the aeration turbulent
shear intensity has been taken into account in the development
of a mathematical model [230]. Theoretical analysis becomes
even more problematical when the complex nature of biomass
mixture (non-Newtonian fluid containing solutes, colloids and
particulates) present in MBRs is taken into account. However,
general anti-fouling phenomena due to aeration occurring in
MBRs can be described.
Basically, the bubbles flowing near to the membrane sur-
face induce local shear transients and liquid flow fluctuations,
increasing back transport phenomenon. The tangential shear at
the membrane surface prevents large particle deposition on the
membrane surface. However, the effect of tangential shear is a
function of particle diameter, with lower shear induced diffu-
sion and lateral migration velocity for smaller particles, leading
to more severe membrane fouling by fine materials [231]. Aer-
ation also affects MBR performance by causing fiber lateral
movement (or sway) in hollow fiber configurations [121]. The
effect of bubbling can help to overcome issues related to high
packing density in hollow fiber bundles. However, it is still a
challenging task for MBR designers to achieve effective aeration
throughout the population of fibers in a bundle [232]. All these
effects, described in more detail elsewhere [104,106,233235],
contribute to a significant reduction in fouling propensity. A
novel explanation for the influence of aeration on MBR foul-
ing has been proposed by Ji and Zhou [174]. According to their
results, aeration rate directly controls the quantity and composi-
tion of the polymeric compounds (EPS) in the biological flocs,
and ultimately the ratio of protein/carbohydrate deposited on the
membrane surface. However, this mechanism cannot explain the
effects of bubble-induced fouling control observed with model
feeds [121].
An optimum aeration rate, beyond which a further increase
has no significant effect on fouling suppression, was originally
observed by Ueda in 1997 [236], and has been verified in many
occasions since [84,237,238]. During MBR optimization stud-
ies, the limits of the aeration were demonstrated through its effect
on the netflux-ratio (netflux over instantaneous flux calculated
for operation with membrane relaxation or backwashing). In this
case, aeration intensity could not further improve hydraulic per-
formances below the critical netflux-ratio of 0.85. Above this
value, the aeration rate was able to limit, to a certain extend,
the formation of severe fouling [239]. This study revealed that,
for specific conditions, the filtration mode has more effect on
MBR fouling than the changes in aeration rates. Intense aera-
tion rate may also damage the floc structure reducing their size,
and releasing EPS in the bioreactor [174,240]. These phenomena
have been similarly described in the sidestream MBR configura-
tion in which the circulation pump is responsible for the break up
of bacterial flocs [241,242]. However, in a small crossflow cell,
fouling was found to decrease linearly with increasing CFV (up
to 4.5 m/s), and no CFV optimum was observed [243]. Detailed
study of the various calculated hydraulic resistances revealed
that CFV values of 2 and 3 m/s were sufficient to prevent the
formation of reversible fouling in UF (30 kDa) and MF (0.3 m)
systems, respectively. Finally, it was shown that high CFV was
more effective in reducing fouling in the MF rather than in the
UFMBR system. This was confirmed by analysis of the mass,
thickness and density of the fouling layer deposited in/on the
membrane under different operating conditions. This may be
due to the effect of CFV on critical flux of particulates. At a
low CFV of 0.1 m/s, the UF membrane fouled less, being less
susceptible to the particle deposition, whereas at a high CFV
of 3.5 m/s, the majority of particles would not deposit (raised
critical flux) on either membrane. However in current MBRs
generation, the CFV is relatively low which could favor the use
of tighter (UF) membranes.
Determination of the CFV induced by aeration of the mem-
brane surface can be difficult to assess and techniques such
as electromagnetic flow velocity meter [244], particle image
velocimetry [232], constant temperature anemometry [245,246],
have be used for liquid velocity estimation in submerged MBR
reactors. Based on the observed CFV in tap water in the riser
section (CFVtp ) of a internal loop-airlift MBR system, Liu et al.
set up a modified model for calculating the CFV of the aerated
activated sludge (CFVas ) over the membrane surface [237]:
CFVas = 1.406 CFV1.226
tp 0.147 (3)
where is the viscosity of the MLSS, and CFVtp can be esti-
mated from equation given in Liu et al.s earlier publication
[247].
3.3.2. Solid retention time (SRT)
SRT (and consequently the F/M ratio), which ultimately con-
trols biomass characteristics, is probably the most important
operating parameter impacting on fouling propensity in MBRs.
Operating an MBR at higher SRT leads inevitably to increase of
MLSS concentration, but this in itself may not necessary lead to
greater fouling (Section 3.2.3) [248].
Extremely low SRTs (down to 2 days) have been tested
to assess fouling propensity [249]. Not surprisingly, fouling
rate increased nearly 10 times when SRT was lowered from
10 to 2 days (corresponding to F/M ratio from to 0.5 to
2.4 gCOD/gMLVSS/day and MLSS of 7.86.9 g/l). There is no
reason (other than purely research-based work) to run MBRs
at such extreme conditions, and, as a general rule, F/M ratio is
recommended to be maintained below 0.5. Other characteris-
tics of performance at SRT as low as 0.25 day are discussed in
[250]. The reasons suggested for the increased fouling rate at
very low SRT include the increased levels of production of EPS.
It should be noted that an increased F/M ratio could occur during
transients in unsteady operation (Section 3.3.3).
At the other end of the spectrum, the temptation to run MBRs
at extended SRT is great, considering the advantages of this pro-
cess over CASP. Indeed the early MBRs were typically run at
very long SRTs to minimize excess sludge. Studies reporting
operation at infinite SRT are generally bench scale, use syn-
thetic feed (or very finely prefiltered sewage) [212,251254] and
therefore do not take into consideration the accumulation of inert
material in the tank. The progressive accumulation in the MBR
tank of non-biodegradable materials (like hair and lint), which
are not completely removed by the MBR pre-treatment pro-
cesses, undeniably leads to clogging of the membrane module
[255]. The increase in MLSS concentration related to extended
SRT could also result in higher fouling propensity (see Section
3.2.3) even with the aeration raised significantly. Previous exper-
iments revealed an increase of MLSS levels from 7 to 18 g/l and
a decrease of F/M ratio from 0.15 to 0.05 kgCOD/kgMLSS/day
when the SRT was increased from 30 to 100 days. Even after
increasing the aeration rate from 15 to 25 l/min, fouling was
nearly twice as great for the longer SRT conditions [155]. In
this scenario, the increased shear provided to control fouling
could breakup biofloc as well as causing cell lysis. Moreover,
the increase in aeration intensity to keep the high MLSS levels
in suspension and properly oxygenated may not be a sustainable
option for the treatment process. During a 300-day operation of
a pilot-scale MBR without wastage (infinite SRT), the MLVSS
increased steadily from 3 to 15 g/l and both removal efficiency
and membrane performances remained constant. At infinite SRT,
most of the substrate is consumed to ensure the maintenance
needs and the synthesis of storage products. The very low appar-
ent net biomass generation observed can also explain the low
fouling propensity observed for high SRT operation in this study
[253]. These two studies show that extended-SRT-operation does
necessary offer lower fouling; other operating conditions such
as flux and aeration rates would also have a major influence on
fouling propensity. The other difficulty with very high SRT is
the raised viscosity that could attenuate the effect of bubbling.
The effects of SRT on biological parameters like MLSS, SMP,
eEPS concentrations, described in Section 3.2, also reveal the
major impact of this operating parameter on MBR fouling. As
a result, selection of the SRT must be considered very carefully
in order to optimize MBR operation (see Section 4.2.2). Some
studies reported the DOC of the supernatant to be independent
of SRT [252]. The lower fouling generally observed at extended
SRT is partially explained by the lower organic carbon concen-
tration in eEPS rather than in SMP. Overall, it is likely that there
is an optimal SRT, between the high fouling tendency of very
low SRT operation and the high viscosity suspension prevalent
for very long SRT. However, the difficulty related to properly
acclimatize an MBR (pilot) plant to different SRTs and conduct
a fair comparison does not allow the determination of an opti-
mum SRT value. This could also explain the discrepancies in the
SRT effects reported in the literature. Criteria such as designed
rate of sludge and MLSS concentration recommended by the
membrane supplier is more prone to define the working SRT.
This point is further discussed in Section 4.2.2.
3.3.3. Unsteady state operation
Unsteady state such as variations in operating conditions
(flow input/HRT and organic load) and shifts in oxygen supply
have also been defined as additional factors leading to changes
in MBR fouling propensity. In real-world applications, such
unsteady state conditions could occur regularly. In an experiment
carried out with a large pilot-scale MBR, the effects of unstable
flow input and unintentional sludge wastage have been assessed
[217]. Although the level of polysaccharides in the filtrate varied
in a chaotic manner, the concentration of this specific compound
increased before and after each sludge withdrawal. While the
increase after wastage was due to the sudden stress experienced
by cells, increase before sludge withdrawal was explained by the
increasingly high MLSS concentration and the resulting low DO
level in the bioreactor. It was concluded that unsteady operation
changed the nature and/or structure (and fouling propensity) of
the polysaccharide rather than the overall EPS formation, and
therefore could worsen the fouling propensity. These findings
confirmed results previously reported on the effects of transient
conditions in feeding patterns. The addition of a spike of acetate
in the feed water significantly decreased the filterability of the
biomass in an MBR; this was due to the rise in SMP levels
resulting from the feed spike [256].
The effects of starvation conditions on the biological sus-
pension have been assessed by incorporating different substrate
impulses in batch tests [257]. Exogenous phases were followed
by starvation periods, both characterized by the So/Xo ratio
(Eq. (4)). For high So/Xo, multiplication of bacteria cells was
observed, while compound storage, characterized by decrease
of MLVSS and the absence of SMPp production and bacteria
lysis, were obtained at low So/Xo ratio. The low F/M conditions
generally used in MBRs are theoretically close to what would
be considered as starvation conditions. Although the influence
of these operating conditions on MBR fouling have not been
reported, the lower amount of SMPp produced may lead to less
severe fouling propensity:


So F
= HRT (4)
Xo M
with So, the feed substrate concentrate and Xo, the MLVSS
concentration.
The start-up phase can also be considered as unsteady oper-
ation and data collected before biomass stabilization (including
the period necessary to reach acclimatization) may become
relevant in the design of MBRs. Cho et al. [197] reported
temporal changes of the bound EPS levels when the MBR
was acclimated to three different SRTs (8, 20 and 80 days).
As expected (considering the general trends described in
Section 3.2.5), the concentration of eEPS was lower for the
longer SRT (8326 mgTOC/gSS for SRT of 8 up to 80 days,
respectively). More interestingly, an initial latent phase was
observed for which eEPS concentration did not vary signifi-
cantly. However, eEPS levels increased exponentially after 40
days of operation at 8-day-SRT, and after 70 days when the
MBR was operated with an SRT of 20 days. No change in eEPS
was observed during the 80 days of operation at 80-day-SRT.
In another MBR set-up operated at infinite SRT, no significant
changes in SMP concentration during 100 days of operation were
observed, although the MLSS increased from 1.8 to 4.5 g/l in the
meantime [258]. After a latent phase of 30 days, MLSS and SMP
levels started to significantly increase and stabilized by reaching
a plateau after 140 days of operation at infinite SRT (operated for
210 days). In this example, eEPS increased continuously from
day 1 to also reach steady-state on day 140 [251]. Nagaoka and
Nemoto [198] observed a rise of MLSS concentration from 4
to 14 g/l over 100 days (SRT value not given) along with a rel-
atively constant increase in eEPS (from 50 to 250 mg TOC/l).
From these examples and the relationship between eEPS-SMP
and fouling propensity defined earlier, further research on the
exact impact of unsteady states on MBR fouling is required to
implement more sustainable MBR operation. At this point in
time, the evidence points to increased membrane fouling during
unsteady state (particularly when F/M is increasing).
3.4. Fouling mechanisms in MBRs
3.4.1. Constant TMP operation
The current trend in MBR design is to operate at constant flux,
and as a result, very few recent studies report the operation of
MBR at constant TMP. In the MBR, like other membrane filtra-
tion processes at constant TMP, a rapid flux decline is expected to
occur during the initial stages of the filtration. The rate of fouling
then decreases before reaching a plateau. Bae and Tak recently
summarized the hypothetical three-phase-process-mechanisms
for initial cake layer formation occurring in MBR [143]. They
filtered MBR mixed liquor samples at 100 kPa over periods of
up to 5 h with a range of UF membranes. According to these
authors, the main parameter affecting the initial fouling (phase 1)
would be the irreversible deposition of the soluble fraction of the
biomass suspension (presumably SMP). During this phase, the
sludge particles and the colloids would not take part in fouling
since they are supposed to be, respectively, removed by cross-
flow (size effect) and to be in too low a concentration to have
a significant effect on fouling. Deposition of sludge particles
on the membrane surface and in the previously deposited lay-
ers is the main phenomenon occurring during phase 2 when the
flux declines more slowly. Phase 3 is then defined when flux
appears to stabilize, indicating that permeation drag and back
transport have reached equilibrium. Although reduced perme-
ation drag limits further severe fouling, compaction of the cake
layer would play a significant role in the slight increase in filtra-
tion resistance observed during this last phase. As little fouling
still occurs during phase 3, this operation can be maintained dur-
ing a certain filtration period, before cleaning of the membrane
is required. However, in this study, fluxes typically dropped to
about 10 l/m2 h which is less than normal constant flux MBR
operation. It is important to note that in phase 3, two factors
are at work. Firstly, the lowered flow slows down the convec-
tion of foulant; it becomes self-limiting. The other factor is that
once the flux is low, the fouling resistance is high, relative to
the membrane resistance. To see significant further decline (say
by a further 50%) requires the fouling resistance to double. It
becomes increasingly difficult to detect fouling trends by simply
inspecting the flux decline profile.
3.4.2. Constant ux operation
With the constant flux approach, the convection of foulant
does not diminish and fouling phenomena self-accelerates and
can eventually create a sharp increase of TMP. With fouling rate,
and therefore cleaning frequency, increasing with flux, operation
conditions favors the MBR to be run at modest fluxes to limit
fouling severity (Section 4.2.2). As a result, numerous studies
have reported the fouling behavior for long-term MBR filtration
carried out at sub-critical flux. However, these long-term exper-
iments have revealed noticeable fouling for MBRs operated at
sub-critical flux. Since its first reference to MBRs in 2001 [28],
fouling behavior over time is generally characterized by a two-
step pattern. During the first period, a very small TMP rise was
observed. For trials carried out over extended time periods, a
noticeable change in the rate of TMP increase then arises after
some critical time period (Fig. 13). Pollice et al. [32] reviewed
the phenomena and two parameters were introduced as indica-
tors for operation under sub-critical conditions: the critical time
over which the prolonged first step is maintained (tcrit ) and the
fouling rate (dTMP/dt) during that step. Table 6 reports tcrit and
dTMP/dt for recent trials and reveals the long periods of filtra-
tion (up to 1200 h) for which fouling rate can be maintained at
very low values (down to 2 104 kPa/h). The fouling rates for
the high TMP-rise-period have also been reported previously
[148]. Prior to these two filtration-steps generally described
in the literature, a conditioning period has also been observed
[86]. This conditioning period (from now called stage 1) has
not been observed or described as such until recently, but may
be a key aspect of fouling creation in MBRs. The dynamics of
the biomass detachment from the membrane in relation to the
Fig. 13. Long-term filtration for constant flux operation (adapted from [14]).
Table 6 ble for the initial stage of fouling during constant flux operation.
Sub-critical long-term parameters (completed from [32]) Ognier et al. [95] described the rapid fouling phenomena induc-
Flux (l/m2 h) dTMP/dt (kPa/h) tcrit (h) References ing irreversible resistance and taking place in the early stage
17 0.005 >600 [259]
of MBR filtration (in frontal mode, i.e. dead-end operation).
22 0.011 1200 [259] Passive adsorption of colloids and organics has been observed
25 0.024 300 [259] even for zero-flux operation, and before any deposition mech-
30 0.072 250 [259] anism initiates [86]. Another detailed study based on passive
n.a. 0.023 350 [260] adsorption revealed that the hydraulic resistance due to this pro-
20 600 [261]
8 350 [262]
cess was almost independent of tangential shear. In terms of
30 0.036 360 [25] relative hydraulic resistance contribution, the initial adsorption
10 0.036 550 [263] has been reported to account for 202000% of the clean mem-
8 0.03 72 [30] brane resistance (mainly depending on the pore size) [263]. In
7 0.006 96 [14] a more recent study, its contribution to the overall resistance
9 0.004 240 [14]
18 0.104 48 [14]
was found to become negligible once filtration was conducted
12 0.0002 300 [264] [88]. The adsorption propensity (determined with the modified
4 0.013 192 [148] Freundlich isothermal adsorption equation) was also studied in
6 0.031 137 [148] relation to the filtration modes employed in submerged MBRs
8 0.6 74 [148] [265]. As a result, colloid adsorption and initial pore block-
ing [170] of new or cleaned membranes by organics substances
is expected in MBRs. The intensity of this effect depends on
filtration and aeration turbulence has also been rarely reported, membrane pore size distribution and surface chemistry (and
but was recently considered in the formation of a mathemati- especially hydrophobicity) [95] (Sections 3.2.5 and 3.2.6). In
cal model [230]. Based on the recent work reported by Zhang a test cell equipped with direct observation through the mem-
et al. [86], a detailed analysis of the mechanisms and factors brane (DOTM) technology, and with crossflow but zero flux,
involved in these three fouling stages follows and is summa- floc was visually observed to temporarily land on the membrane
rized in Fig. 14. [86]. This was defined as a random interaction process rather
than proper cake formation phenomenon. While some flocs were
3.4.2.1. Stage 1conditioning fouling. As in constant TMP seen to roll and slide across the membrane, biological aggregates
operation, strong interactions between the membrane surface typically detached and left a residual footprint of smaller flocs
and the EPS present in the mixed liquor are probably responsi- or EPS material. Biomass approaching the membrane surface

Fig. 14. Fouling mechanisms for MBR operated at constant flux (adapted from [86]).
was then able to attach more easily to the membrane, colonize
the separation surface and contribute to stage 2.
3.4.2.2. Stage 2slow (steady) fouling. Even though MBRs
are operated below the critical flux for the biomass, biofloc may
randomly land (see above) and contribute to the second foul-
ing stage. After stage 1, the membrane surface is expected to
be mostly covered by SMP, leading to the higher attachment
propensity of biomass particles and colloids. Because of the low
critical flux determined for SMP species, further adsorption and
deposition of organics on the membrane surface may also occur
during stage 2. Since adsorption may take place not only at the
membrane pores but also on the whole surface, biological flocs
may initiate cake formation without directly affecting the perme-
ability in this stage. Over time, this phenomenon would worsen.
The rate of EPS deposition, and resulting TMP rise, is expected
to increase when the operating flux is higher, leading to a shorter
stage 2 operation (Table 6). The fouling mechanisms described
above would prevail even with a good hydrodynamic environ-
ment that provides adequate surface shear over the membrane
surface. However as maldistributions of flow, shear or flux are
generally expected in MBRs, irregular fouling patterns can be
anticipated.
3.4.2.3. Stage 3TMP jump. With regions or pores of the
membrane more fouled than others, flux is expected to sig-
nificantly decrease in those specific locations. As a result, the
overall permeate productivity redistributes to the less fouled
membrane areas or pores, for which local flux increases (see
Section 2), exceeding a critical flux (defined as sustainable flux
in Section 4.2.2). These phenomena have a self-accelerating
nature and severe fouling, characterized by an exponential
TMP increase, is generally obtained if the filtration is main-
tained. The sudden rise in TMP or jump is a consequence
of constant flux operation and several mechanisms can be pos-
tulated for the rapid increase in TMP at a given condition
[86]:
(i) The inhomogeneous fouling (area loss) model. This model
was proposed to explain the observed TMP profiles in nom-
inally sub-critical filtration of upflow anaerobic sludge [25].
The TMP jump appeared to coincide with a measured loss
of local permeability at different positions along the mem-
brane, due to slow fouling by EPS. It was argued that the
flux redistribution (to maintain the constant average flux)
resulted in regions of supra-critical flux and consequently
in rapid fouling and TMP rise.
(ii) The inhomogeneous fouling (pore loss) model. Similar TMP
transients have been observed for the crossflow MF of a
model biopolymer (alginate) [17]. These trends revealed
that the TMP transient can occur with relatively simple
feeds. The data obtained have been explained by a model that
involves flux redistribution among open pores, allowing for
the pore size distribution. Local pore velocities eventually
exceed the critical flux of alginate aggregates that rapidly
block the pores. This idea was also the basis of the model
proposed by Ognier et al. [31]. While the area loss model
considers macroscopic redistribution of flux, the pore loss
model focuses on microscopic scale. In MBR systems, it is
expected that both mechanisms occur simultaneously.
(iii) The critical suction pressure model. Using a fine colloid,
filtered in dead-end mode, onto an immersed hollow fiber,
gradual TMP rise followed by a rapid increase in TMP was
observed. Both autopsy and modeling suggested a critical
suction pressure at which coagulation occurs at the base
of the cake [266]. The very thin dense layer observed next
to the membrane confirmed the rapid increase in resistance
leading to the TMP jump. Although this model was obtained
with dead-end rather than crossflow operation, there is no
reason why this mechanism could not apply to sidestream
or submerged MBRs. A requirement for that model is that
fouling continues to occur over time until the critical suction
pressure is reached, and that the deposit compound(s) have
the potential to coalesce or collapse. Biofilms and deposit
layers in MBRs are likely to have this tendency.
(iv) Percolation theory. According to percolation theory, the
porosity of the fouling layer gradually reduces due to the
continuous filtration and material deposition within the
deposit layer. At a critical condition, the fouling cake loses
connectivity and resistance, and TMP, increase rapidly. This
model has been proposed for MBRs [34], but the model indi-
cates a very rapid change (within minutes), which has not
been observed in practice. However, it is plausible that the
percolation theory approach, combined with the inhomo-
geneous fouling (area loss) model, could satisfy the more
gradual kinetics of the typical TMP transient. Similarly,
fractal theory was successfully applied to describe cake
microstructure and properties and to explain the cake com-
pression observed during MBR operation [267].
(v) The inhomogeneous ber bundle model. Another manifes-
tation of the TMP transient has been observed for model
fiber bundles where the flow from individual fibers was
monitored [118]. The bundle was operated under suction
at constant permeate flow, giving constant average flux, and
initially this was evenly distributed amongst the fibers. How-
ever over time, the flows became less evenly distributed so
that the standard deviation of the fluxes of individual fibers
started to increase from the initial range of 0.10.15 up to
0.4 l/m2 h. Consequently, the TMP rose to maintain the aver-
age flux across the fiber bundle, mirroring the increase in
the fluxes standard deviation. At some point both TMP and
standard deviation showed a rapid rise. This is believed to
be due to flow maldistribution within the bundle leading
to local blockages between fibers and membrane fouling. It
was possible to obtain more steadily TMP and standard devi-
ation profiles when the flow regime around the fibers was
more vigorous (higher liquid and/or air intensity). Although
this trend was observed for a small model bundle, the phe-
nomena are likely to occur in larger bundles.
The mechanisms (i)(v) listed above are all self-accelerating
and this is a feature of stage 3 fouling. It is probable that more
than one of these mechanisms apply simultaneously when an
MBR reaches the TMP jump condition.
4. Mitigation of MBR fouling
4.1. Removal of fouling
4.1.1. Physical cleaning
Physical cleaning techniques for MBRs include mainly mem-
brane relaxation (where filtration is paused) and membrane
backwashing (where permeate is pumped in the reverse direction
through the membrane). These techniques have been incorpo-
rated in most MBR designs as standard operating strategies to
limit fouling; although vigorous backwashing is not an option
for flat plate submerged membranes.
Backwashing (also called backflushing) has been found to
successfully remove most of the reversible fouling due to pore
blocking, transport it back into the bioreactor, and partially dis-
lodge loosely attached sludge cake from the membrane surface.
In some cases, clogging near the membrane surface may also be
partially loosened or removed by backwashing. The efficiency of
backwashing has been studied in detail [268270]. Key parame-
ters in the design of backwashing are its frequency, duration, the
ratio between those two parameters and its intensity. For exam-
ple, less frequent, but longer backwashing (600 s filtration/45 s
backwashing) was found to be more efficient than more fre-
quent backwashing (200 s filtration/15 s backwashing) [170]. In
another study based on factorial design, suction time (between
8 and 16 min) was found to have more effect on fouling removal
than both the aeration intensity (0.30.9 m3 /m2 h) and the back-
wash time (2545 s) [239]. Although more fouling is expected
to be removed when backwashing duration and frequency are
increased, optimization of backwashing is required in regard to
energy and permeate consumptions. This was achieved by the
design of a generic control system which automatically opti-
mized the duration of the backwash according to the monitored
value of TMP [271].
This anti-fouling operation obviously affects operating costs
as energy is required to achieve a pressure suitable for flow rever-
sion. Moreover, between 5 and 30% of the produced permeate
is used in the process. Comparison between submerged hollow
fiber and flat sheet MBR revealed the slightly higher overall
flux obtained when operating the membrane constantly at low
flux [108]. In this example, flat sheet membranes, which can-
not be backwashed, were operated constantly with flux ranging
between 20 and 27 l/m2 h. The hollow fiber MBR was operated
at higher flux (2333 l/m2 h) but with 25% of the permeate prod-
uct being recycled for backwashing (45 s of backwashing after
every 600 s of operation).
Air can also be used as the backflushing medium [272].
Although improving the flux by nearly 400% (compared to con-
tinuous operation), 15 min of air backwash was required every
15 min of filtration to obtain this result [273]. However, air back-
washing is an efficient method for flux recovery, it may also
present potential issues of membrane breakage and rewetting.
Membrane relaxation (or non-continuous operation of the
membrane) significantly improves membrane productivity.
Under relaxation, back transport of foulants is naturally
enhanced as non-irreversibly attached foulants can diffuse away
from the membrane surface through the concentration gradi-
ent. The fouling removal efficiency of this method can be fur-
ther increased when air scouring is applied during relaxation
[149,274]. Detailed studies of the TMP behavior during this
type of operation revealed that although the fouling rate is gen-
erally higher than for continuous filtration, membrane relaxation
allows filtration to be maintained for longer period of times
before the need for cleaning [207]. Although some have reported
that this type of operation may not be economically feasible for
large-scale MBRs [149], further cost and productivity analysis
are probably required to compare this method against backwash-
ing. Recent studies assessing alternative strategies for fouling
mitigation tend to combine intermittent operation with frequent
backwashing for optimum results [137,275].
4.1.2. Chemical cleaning
It is expected that membrane relaxation and backwashing
effectiveness tend to decrease with operation time as more irre-
versible fouling accumulates on the membrane surface. There-
fore, in addition to the physical cleaning strategies, differ-
ent types/intensities of chemical cleaning may also be recom-
mended. They include:
Chemically enhanced backwash (on a daily basis),
Maintenance cleaning with higher chemical concentration
(weekly), and
Intensive (or recovery) chemical cleaning (once or twice a
year).
Maintenance cleaning is used to maintain design permeability
and helps to reduce the frequency of intense cleaning. Intensive
cleaning is generally carried out when further filtration is no
longer sustainable because of an elevated TMP. Each of the four
main MBR suppliers (Kubota, Memcor, Mitsubishi and Zenon)
proposes their own chemical cleaning recipes, which differ
mainly in terms of concentration and methods (Table 7). Under
normal conditions, the prevalent cleaning agents remain sodium
hypochlorite (for organic foulants) and citric acid (for inorgan-
ics). Sodium hypochloride hydrolyzes the organic molecules,
and therefore loosen the particles and biofilm attached to the
membrane. The effects of cleaning chemical agents like NaOCl
on microbial community have been also recently studied for
modeled MBR processes [276]. It is also common for MBR
suppliers to adapt specific protocols for chemical cleanings (i.e.
chemical concentrations and cleaning frequencies) for individ-
ual facilities [115,179,255]. It also has been mentioned that the
level of pollutants (measured as TOC) in the permeate rises just
after the chemical cleaning episodes [115]. This is important for
MBRs used in reclamation process trains (i.e. upstream of RO
for example). So far, no systematic studies on cleaning agents
or procedures have been published [277]. This is probably due
to the site-specific nature of the MBR fouling.
Maintenance cleaning, taking up to 30 min for a complete
cycle, is normally carried out every 37 days at a moderate
reagent concentration of 0.01 wt.% NaOCl. Recovery cleaning
employs rather higher reagent concentrations of 0.20.5 wt.%
NaOCl coupled with 0.20.3 wt.% citric acid or 0.51 wt.%
oxalic acid (Table 7).
Table 7
Intensive chemical cleaning protocols for four MBR suppliersa (from [255])
Type Chemicals
NaOCl
Mitsubishi CIL
Citric acid
NaOCl
Zenon CIP
Citric acid
NaOCl
Memcor CIP
Citric acid
NaOCl
Kubota CIL
Oxalic acid
CIL: cleaning in line where chemical solutions are generally backflow (under gravity) inside the membrane. CIP: cleaning in place where membrane tank is isolated
and drained; the module is rinsed before being soaked in the cleaning solution and rinsed to remove excess of chlorine.
a The exact protocol for chemical cleaning can vary from a plant to another.
Research on the efficiency of sonification for removing cake
layers in MBRs has also been carried out [96]. The sonifica-
tion cleaning process is based on the breakdown of the fouling
cake into smaller fragments. Although sonification can success-
fully remove the cake from the membrane surface, this cleaning
method was not effective on all types of fouling due to pore
blocking and may even worsen this type of fouling. A combi-
nation of sonification with backwashing and chemical cleaning
appeared to achieve almost complete flux recovery [278]. More
details of the cleaning mechanisms are available in [278]. How-
ever, sonification would be difficult to apply at a large-scale due
to the focused nature of the sonic energy.
4.2. Limitation of fouling
It may also be possible to prevent fouling before its occur-
rence by (1) improving the anti-fouling properties of the mem-
brane, (2) operating the MBR under specific non-or-little-
fouling conditions and/or (3) pre-treating the biomass suspen-
sion to limit its fouling propensity.
4.2.1. Optimization of membrane characteristics
In MBRs, chemical modifications of the membrane surface
have been shown to efficiently improve anti-fouling proper-
ties. As mentioned above (Section 3.1.2), more severe foul-
ing is expected when hydrophobic membranes are used in the
MBR, and efforts have been focused on increasing membrane
hydrophilicity through membrane modification. Recent exam-
ples for MBRs comprise NH3 and CO2 plasma treatments of
polypropylene hollow fibers [128,129]. In both cases, X-ray
photoelectron spectroscopy (XPS) and SEM were used to char-
acterize the structural and morphological nature of the modi-
fied membrane surface. With the introduction of polar groups
(from oxygen and nitrogen) on the membrane surface, mem-
brane hydrophilicity significantly increased and new membranes
presented better filtration performances and flux recovery than
those of unmodified membranes. In another study, the addition
of TiO2 nanoparticles to the casting solution and a precoat of
TiO2 allowed the preparation of two types of TiO2 -immobilized
UF membrane (entrapped and deposited, respectively), which
were also used in MBR systems [143,279]. As a result, lower
Concentration (%) Protocols
0.3
Backflow through membrane (2 h) + soaking (2 h)
0.2
0.2
Backpulse and recirculate
0.20.3
0.01
Recirculate through lumens, mixed liquors and in-tank air manifolds
0.2
0.5
Backflow and soaking (2 h)
1
flux decline was obtained with the TiO2 -membranes compared
to that of unmodified membranes.
As it was possible to add a larger amount of TiO2 parti-
cles on as a precoat to a membrane, this filter showed greater
fouling mitigation compared to that of the TiO2 -entrapped-
membrane. Similarly, when MBR membranes were precoated
with ferric hydroxide flocs and compared to an unmodified
MBR, both effluent quality and productivity were found to
increase [280]. This phenomenon was explained by the adsorp-
tion of soluble organics on ferric hydroxide flocs, limiting the
direct contact between the organics and the membrane. Finally,
fouling phenomena have been used to investigate the creation
of self-forming dynamic membrane coupled bioreactors [281].
By using coarse pore-sized substrates and allowing cake and
gel layers to deposit on the surface, a self-forming membrane
developed with a high flux and good removal efficiencies. How-
ever, because of the nature of the filtration barrier, the effluent
quality cannot be guaranteed, and this is of concern in many
applications.
4.2.2. Optimization of operating conditions
4.2.2.1. Aeration. Since the energy involved in providing aer-
ation to the membrane remains a significant cost factor in MBR
design, efforts have been focused on optimization of air flow-
rate. The specific design of airflow patterns and location of
aerators have also been defined as crucial parameters in foul-
ing mitigation. Recent developments in aeration design carried
out by MBR suppliers are often reported in patent format, and
involve cyclic aeration systems [282], and improved aerator sys-
tems [283,284] for example. A recent study reported a detailed
comparison of various aeration devices used in tubular mem-
branes. The results indicated that complex aeration systems with
multiple orifices injecting air homogeneously in the feed flow
featured the highest performances [285]. As mentioned before,
the effect of aeration varies from hollow fiber to flat plate mem-
brane configurations. The presence of a bi-chamber (riser and
down-comer) in a Kubota MBR plays a significant role in induc-
ing high CFV [244]. In the same study, lower uplift resistance
and higher CFV were induced by uniformly distributed fine
air bubbles (issued from a porous media with 0.5 mm holes)
compared to performances obtained with large bubbles (from
2 mm hole diffuser) at similar aeration rates. The air/permeate
ratio (m3 /m3 ) can also be a useful parameter to characterize the
intensity of aeration required to obtain a given amount of treated
water. Values given by MBR suppliers may vary between 24 and
50, depending of the membrane configuration (flat sheet versus
hollow fiber) and the MBR tank design (membrane and aerobic
zone combined into one tank or not) [115]. Preliminary work
carried out in Singapore on large-scale MBRs revealed these
original ratios to be quite conservative, since it was possible
to decrease them (down to 56% of their original value) with-
out significant fouling increase [115]. Attempts to increase the
critical flux in submerged MBR by varying the aeration rates
has been reported [286]. In order to minimize fouling during
high throughput operation, aeration was increased and returned
to lower values for the low throughput period. Based on these
short-term experiments, it was possible to use this technique to
minimize energy consumption. However, a recent study from
Choi et al. [88] carried out with a crossflow MBR device, indi-
cates the tangential shear to have no effect on flux decline when
pseudo steady-state is reached. In other words, increasing CFV
does not decrease fouling intensity when the deposition layer
starts to govern the permeate flux behavior. In the absence of
CFV, flux decline was predominantly caused by reversible foul-
ing, while slightly higher irreversible fouling was detected when
CFV was applied [88].
The intermittent operation of aeration has also been reported
for (de)nitrification MBR systems [198,287]. In this uncommon
scenario of single tank MBR used for both anoxic and aerobic
biological degradation, filtration is carried out during the aerobic
phase to take advantage of the anti-fouling properties of the air
scouring. While some authors testing intermittent aeration do not
recommend this type of operation as severe fouling was observed
as soon air sparging ceases [170,238], others have reported that
efficient fouling control was achieved by intermittent bubbling
[288,289]. Pulsing air at a frequency of 1 s on/1 s off allowed an
improvement in operating flux ranging from 20 to 100% and was
found more efficient than lower frequencies (510 s on/510 s
off) more conventionally applied in the industry [288]. However,
such system may require the operation of a robust activators and
valves at these high frequencies and may not be economically
practical.
4.2.2.2. Other operating conditions. As mentioned before
(Section 3.3.2), SRT remains probably the main operating
parameter defining the characteristics of the biomass suspension
and its fouling propensity. With the numerous reports defining
the relation between SRT and concentrations of both eEPS and
SMP, it appears that the overall performance of the MBR is
closely related to the choice of SRT value. Further optimiza-
tions of operating conditions through reactor design have been
studied and include the addition of a spiral flocculator [290],
vibrating membranes [291], helical baffles [292], suction mode
[97] and high performance compact reactor [293], novel types
of air lift [104], porous and flexible suspended membrane car-
riers [294] and the sequencing batch MBR [295] for example.
Finally, the membrane module design remains another impor-
tant parameter in the optimization of the MBR operation, and
more precisely, the use of air sparging. In a specially designed
module in which air bubbles were confined in close proximity
to the hollow fiber (rather than diffusing in the reactor), higher
permeability was obtained [296].
4.2.2.3. Sustainable ux. The energy demand for operation is
a potential weakness for the future development of the MBR
process. It is recognized that the energy usage of MBRs is still
higher than conventional activated sludge systems due to the
need to control membrane fouling by different strategies. At
the end of the day, MBRs can be economically viable only if it
delivers a reasonable flux rate without significant fouling. Since
permeation rate and fouling decrease simultaneously, most MBR
systems operate at low fluxes to limit rapid and severe membrane
fouling. The concept of sustainable flux in MBRs can be defined
as the flux for which the TMP increases gradually at an accept-
able rate, such that chemical cleaning is not necessary [207]. The
rate of TMP increase and the period of filtration before chemi-
cal cleaning is required are left to the operators discretion, and
therefore a more detailed definition of sustainable flux cannot
be possible. While critical flux was mainly determined during
short-term experiments, sustainable flux can only be assessed
through longer filtration periods. However, sustainable flux can
also be defined as sub-critical flux by default. In such a system,
not only the flux value is of importance but also the strategies
used to maintain this given flux.
4.2.3. Modication of biomass characteristics
4.2.3.1. Coagulant/occulent. Ferric chloride and aluminum
sulfate (alum) are two types of coagulant commonly used for
water and wastewater treatments. Both have been added to
reduce significantly membrane fouling in MBRs. Once dis-
solved in water, alum forms hydroxide precipitates which adsorb
materials such as suspended particles, colloids and soluble
organics. In MBR-based trials, the addition of alum led to
a significant decrease of the SMPc concentration, along with
an improvement in membrane hydraulic performances [297].
Because of back transport and shear induced fouling control
mechanisms, large microbial flocs are expected to have a lower
impact on membrane fouling. The permeability enhancement
observed for hybrid coagulant/MBR systems are therefore due to
the largest flocs formed. A recent MBR-based example reported
that small biological colloids (from 0.1 to 2 m) coagulated and
formed larger aggregate when alum was added to MBR acti-
vated sludge [298]. Although more expensive, ferric chloride
was found to have higher efficiency than that of alum. Zeolite has
also been used in MBRs and allowed the creation of rigid flocs
that have lower specific fouling resistance. Further details about
the mechanisms of performance enhancement due to zeolite and
alum can be obtained from [298]. The addition of ferric iron has
also been tested on an MBR for enhancing the production of iron-
oxidizing bacteria, responsible for the degradation of gaseous
H2 S. In this study, specific ferric precipitate like ferric phos-
phate and K-jarosite (K-Fe3 (SO4 )2 (OH)6 ) have been observed
to foul the membrane [299]. Pre-treatment of the effluent is also
possible and studies based on the pre-coagulation/sedimentation
of effluent before its introduction in the bioreactor revealed the
fouling limitation offered by this technique. Obviously, pre-
treatment of the feed is a crucial step in the MBR process.
Fundamental of sieving, current state-of-the-art mechanical pre-
treatment and results from the comparison between different
types of sieves are given in [300]. In a recent example, the addi-
tion of iron based coagulant controlled both irreversible fouling
and suspension viscosity [145]. Ferric hydroxide flocs have also
been used in the MBR process as a membrane pre-coating agent.
Not only the specific flux of this set up was higher, but the efflu-
ent quality was also improved compared to the non-coated MBR
system [280]. In this study, additional ferric chloride was added
to successfully remove the non-biodegradable organics which
accumulated in the bioreactor. This operation also led to a rapid
increase in membrane specific flux.
4.2.3.2. Adsorbent agents. Addition of adsorbents into biologi-
cal treatment systems decreases the level of pollutants, and more
particularly organic compounds. When PAC is mixed with the
MBR biological suspension, biologically activated carbon forms
and is responsible for significant uptake of soluble organics. Dur-
ing long-term runs, PAC gradually incorporates to the biofloc
to form some biologically activated carbon [301]. Adsorption
of EPS on PAC has been studied during the comparison of
sidestream and submerged hybrid PAC-MBRs [302]. For this
reason, lower fouling propensity is expected in MBR processes
when biomass is mixed with adsorbents. Results conducted with
only MBR supernatant also clearly revealed lower fouling when
PAC was added (up to 1 g/l) [303]. An optimum PAC concen-
tration of 1.2 g/l was obtained for filtration of activated sludge
[262]. In this study, floc size distribution and apparent viscosity
of the biomass were the main factors responsible for the lower
cake resistance observed when PAC was added to the bioreactor.
However, no significant improvement of filtration was obtained
with the addition of 5 g/l of PAC and no sludge wastage [207]. It
was postulated that the originally introduced-PAC was quickly
saturated with organic pollutants. Only the regular addition of
PAC into the bioreactor showed good fouling limitation, as the
system was operated at lower SRT. Results reported by Fang et al.
[304] confirmed this hypothesis as virgin PAC was responsible
for 22% reduction of the filtration resistance, while pre-sorbed
PAC only reduced the resistance by 14%.
Finally, a detailed mathematical model considering sub-
processes like biological reactions in the bulk liquid solution,
film transfer from bulk liquid phase to the biofilm, diffusion with
biological reaction inside biofilm, adsorption equilibrium at the
biofilmadsorbent interface, and diffusion within the PAC par-
ticles has been proposed for predicting performances for hybrid
PAC/MBR systems [305]. Numerous other studies reported the
use of PAC for MBR fouling limitation, but generally failed to
assess key issues such as extra operating cost and disposal of
the elevated amount of sludge to be wasted. However, Ng et al.
recently assessed more clearly the long-term performances of
such hybrid systems [301].
In order to obtain higher biological aggregates in the biore-
actor, aerobic granular sludge has also been used in MBR sys-
tems [144]. With an average size around 1 mm, granular sludge
increased the membrane permeability by 50%, but lower clean-
ing recoveries were observed (88% of those obtained with a
conventional MBR).
A novel membrane performance enhancer (MPE 50) has been
recently developed by Nalco and applied to MBRs. When 1 g/l
of cationic polymer-based compound was added directly to the
bioreactor, SMPc was found to decrease from 41 to 21 mg/l
[306]. The interaction between the polymer and the soluble
organics in general, and SMPc in particular, was named as the
main mechanism responsible for the performance enhancement
when Nalcos polymer was used. In another example, an MBR
operated with MLSS as high as 45 g/l featured a lower fouling
propensity when 2.2 g/l of polymer was mixed to the bioreactor.
Experiments conducted with different system configurations
of submerged hollow fiber membranes allowed direct compar-
ison of hydraulic performances for pre-flocculation and PAC
addition. Under the operating conditions used in this study, pre-
flocculation presented higher fouling mitigation than that of PAC
addition [290]. However, when both strategies were used simul-
taneously, membrane performances were maximum [290,307].
5. Conclusions
After more than 10 years of intensive research, consensus
on the exact fouling phenomena in MBRs has not been reached
yet. Originally, it was suspected that aeration rate and MLSS
concentration had the main impact on MBR fouling. Notwith-
standing their significant effects, new areas of research have
been since developed around the more detailed characterization
of these parameters. Efforts now concentrate on optimizing air
distribution along the membrane modules and on more precise
identification of the biological parameters, which have the most
influence on the membrane performances. With the significant
changes in biomass characteristics from one plant to another, it
is not surprising to observe different biomass parameters affect-
ing MBR fouling with various propensities. These disparities
are also partly due to the different analytical methods and instru-
ments used in the reported studies. In other words, the quest for a
single fouling parameter in MBR seems in vain. A large number
of recent publications indicate the biomass supernatant (SMP)
and its carbohydrate fraction to be one of the main parameters
affecting MBR fouling. However, the more detailed characteri-
zation of the supernatant and the fouling layer currently carried
out also reveals the significant role played by the protein fraction.
The effect of pore size on membrane fouling is also crucial for
MBR design, but the assessment of an optimized membrane pore
size is time-dependant. MF-based MBR systems seem to rely on
initial fouling and the resulting creation of a dynamic membrane
to produce high product quality, while UF-based MBRs feature
good rejection from the early stage of filtration. However, this
review revealed no clear advantage of using tight membranes
over more open pores (within a given flux range). Finally, the
filtration time (short-term versus long-term), the mode of opera-
tion (constant flux versus constant TMP), the initial stage of the
membrane (new versus cleaned), the operating conditions and
the cleaning protocol are also crucial elements when the foul-
ing experiments are designed and should be carefully selected,
reported and analyzed in view of the results. The critical flux
concept and its determination with the flux-stepping experiment
remains an interesting tool to assess fouling propensity for a
mc cake load/membrane area (kg/m2 )
given operating condition, but cannot be used for long-term fil-
MALDI-MS matrix-assisted laser desorption ionization
tration predictions. Instead, the concept of sustainable flux, for
mass spectrometry
which filtration can be maintained over an extended period of
MBR membrane bioreactor
time, is more appropriate for real MBR plants. Effectiveness
MF microfiltration
and strategies for physical and chemical cleanings are under-
MLSS mixed liquor suspended solids (g/l)
reported in the open literature, and there are still opportunities
MLVSS mixed liquor volatile suspended solids (g/l)
to match cleaning protocols with the foulant species present.
MW molecular weight
At this stage in time, it is difficult to propose a short-listing of
MWCO molecular weight cut-off (kDa)
all the parameters which could predict and/or model MBR foul-
NOM natural organic matter
ing. The large number of studies published on the subject and
PAC powdered activated carbon
reviewed in Section 3 reveals the complex interactions existing
Rc hydraulic resistance attributed to the cake layer
between the different fouling parameters. Further understand-
(m1 )
ing of the nature of MBR foulants and their interactions with
Rcol hydraulic resistance attributed to colloid species
the membrane material may provide new directions for clean-
(m1 )
ing agents and protocols, and fouling mitigation strategies for
Rm hydraulic resistance of the membrane (m1 )
MBRs. In that effort, previous studies reported for flocculation,
Rp hydraulic resistance attributed to pore blocking
settling and dewatering of activated sludge can be used as inter-
(m1 )
esting parallels.
Rsol hydraulic resistance attributed to soluble species
(m1 )
Acknowledgments Rss hydraulic resistance attributed to the suspended
solids (m1 )
The authors gratefully thank the Australian Research Council Rsup hydraulic resistance attributed to the biomass
and the NewSouth Global Postdoctoral Fellowship Program for supernatant (m1 )
the financial support of this study, and Prof Simon Judd, Dr. Yun Rt total hydraulic resistance (m1 )
Ye and Ms. Yulita Marselina for their contribution to this review. SMP soluble microbial products (mg/l)
SMPc fraction of carbohydrate contained in the sludge
solution (mg/gSS)
Nomenclature SMPp fraction of protein contained in the sludge solution
(mg/gSS)
BPC biopolymer clusters
So substrate concentration (g/l)
BSA bovin serum albumin
SRT solid retention time (day)
CASP conventional activated sludge process
SUVA specific ultra violet absorbance (m l mg/C)
CFV crossflow velocity (m/s)
t temperature ( C)
CFVas crossflow velocity of activated sludge (m/s)
tcrit critical time over which step one is maintained (h)
CFVtp crossflow velocity of tap water (m/s)
TMP transmembrane pressure (mbar)
COD chemical oxygen demand (mg/l)
TOC total organic carbon (mg/l)
CST capillarity suction time (s)
UF ultrafiltration
dTMP/dt rate of TMP increase (or fouling rate) (kPa/h)
UG gas superficial velocity (m/s)
DO dissolved oxygen (mg/l)
UL liquid superficial velocity (m/s)
DOC dissolved organic carbon (mg/l)
V cumulative volume of permeate
DOTM direct observation through membrane
Xo MLSS concentration (g/l)
eEPSc fraction of carbohydrate contained in extracted
solution from sludge (mg/gSS) Greek symbols
eEPSp fraction of protein contained in extracted solution c cake specific resistance (m/kg)
from sludge (mg/gSS) dynamic viscosity of MLSS (mPa s)
EPS extracellular polymeric substances (mg/gSS)
F/M food to microorganisms ratio
HPSEC high performance size exclusion chromatography References
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Glossary
Adhesion: Molecular attraction between materials. In membrane separation
processes, mechanisms include mechanical (interlocking), chemical (ionic,
covalent or hydrogen bonding) and dispersive (adsorption, van der Waals
force) adhesions.
Biolm: Complex aggregation of microorganisms on a solid surface. This phe-
nomenon is possible thanks to the excretion of the protective and adhesive
EPS.
Biofouling: Combination of biofilm formation and bacterial adhesion and depo-
sition on the membrane surface.
Biological oc: Aggregation of bacteria thanks to the EPS action. The relatively
large floc size (few hundred micrometers) allows the biomass settlement in
CASP.
Biomass: Microorganisms and other biological solid materials growing in the
bioreactor. Biomass concentration can be characterized by the mixed liquor
volatile suspended solids (MLVSS) concentration.
Biomass supernatant: Solution generally obtained after centrifugation (and/or
filtration) of the activated sludge biomass. The supernatant is composed by
colloidal and soluble species.
Bioreactor: Tank designed to biologically treat wastewater by the use of biomass.
Carbohydrate: Chemical compounds made of hydrogen, carbon and oxygen,
such as sugars, starches, and cellulose. Polysaccharides are one type of car-
bohydrate prevalent in MBRs.
Colloids: Very small, finely divided solids (particles that do not dissolve) that
remain dispersed in the aqueous phase due to their small size (from 1 nm to
1 m) and electrical charge.
Conventional Activated Sludge Process (CASP): Process in which a clarifier
follows the aeration tank and is used for solids separation.
Deposition: Settling of particles from a solution or suspension mixture on a
pre-existing surface.
Extracellular polymeric substances (EPS): Construction materials for microbial
aggregates such as biofilms, flocs and activated sludge liquors (see Section
3.2.5).
Extracted extracellular polymeric substances (eEPS): Solution obtained after
the physical and/or chemical extraction of the EPS from the biological walls
of the microorganisms.
Fouling: Undesirable accumulation of (particulate, colloidal, molecular) mate-
rials on the internal or external structure of the membrane. If the fouling
involves living things such as microorganisms, the term biofouling may be
used.
Hydraulic retention time (HRT): The HRT is equivalent to the theoretical deten-
tion time for an ideal plug flow or completely mixed reactor and is calculated
as the volume of bioreactor divided by the influent flowrate.
Membrane bioreactor (MBR): Technology combining biological degradation
process by activated sludge with a direct solidliquid separation by filtration.
Proteins: Chemical substances based on the polymerisation of amino acids. Dur-
ing biological degradation, proteins are hydrolysed to polypeptides, amino
acids, and then ammonia and simple organic compounds.
Solids residence time (SRT): The SRT (also called the mean cell residence time
or sludge age) is equivalent to the average time that microorganisms spend
in the MBR and is calculated as the mass of organisms in the reactor divided
by the mass of organisms generated/wasted from the reactor each day.
Soluble microbial products (SMP): SMP (also called soluble EPS or biomass
supernatant) are defined as soluble cellular components that are released
during cell lysis, diffuse through the cell membrane, are lost during synthesis
or are excreted. In MBR systems, they can also be provided from the feed
substrate (see Section 3.2.6).