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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.
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
Cake filtration Boundary layer resistance Deposit of particles larger than the membrane pore size onto the t/V = AV + B
membrane surface
Complete blocking Pore blocking Occlusion of pores by particles with no particle superimposition ln(J/J0 ) = At + B
Intermediate blocking Long-term adsorption Occlusion of pores by particles with particle superimposition 1/J = At + B
Standard blocking Direct adsorption 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 The reason for such behavior is that for very small parti-
membrane. cles, inter-particle repulsion (electrostatic repulsion) exerts a
While fouling is generally observed as being slower in con- dominant effect on the voidage of the cake layer. In this range
stant flux operation, there is some evidence that the deposition of particle size, the inter-particle repulsion decreases with the
under these low fouling conditions may be more irreversible as increase in particle size resulting in the decrease of permeability
the resultant mechanism tends to be predominately internal foul- [40]. After a certain value of particle size, the effect of the elec-
ing by macromolecular species. Constant flux operation may trostatic force becomes negligible and the permeability increases
generate a substantial initial deposit, but its effect on subse- with the increase in particle size. Fane et al. [41] observed a
quent deposition of macromolecules may be beneficial in some similar dependency of the permeability of the cake layer on
circumstances by serving as a prefilter for species which may particle size. They proposed a different explanation based on
otherwise infiltrate more deeply into the membrane pores. In the counter balance of the Brownian diffusion (dominating for
addition, the constraints of productivity in terms of flux and per- smaller particles) and particle migration due to hydrodynamic
meation of targeted species for applications such as fermentation forces (dominating for larger particles).
redefine the optimal flux operational mode. The development of the cake layer during microfiltration
Intermittent filtration combined with continuous crossflow was also studied [4247]. Cakes formed in the crossflow mode
may allow deposits to relax as long as the particles are still labile. may have higher specific cake resistances than cakes formed in
In appropriate regions suggested by Bacchin et al. [19] where dead-end filtration and may even increase with the increase in
coagulation or aggregation has not occurred, this approach may membrane resistance [48]. Many of these observations can be
allow removal of foulant cakes. However, for many biological explained by size dependent particle deposition and the depen-
solids, the cohesive strength of the cake may be significant and dence of the specific resistance on the particle size. Based on the
proteins adsorption and gel formation result in strong attractive mass transfer mechanisms, there is a maximum diameter of par-
bonds to the membrane materials. 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-
2.3. Cake structure and the effect of mixed species on cake cific resistance may increase. In addition, cake formation during
morphology crossflow tends to eliminate larger particles from the deposits,
leading to cake containing a finer fraction of the particle size
Once the cake is formed on the membrane surface, the cake distribution. Plugging and catastrophic reduction in permeabil-
layer offers an additional resistance for filtration. The perme- ity of the retained cake is another potential cause of the two
ability of the cake layer can be affected by flux, electrostatic stage TMP increase during sub-critical flux operation indicated
interactions, and particle size. General observations by Petsev earlier [34]. However, Keskinler et al. [44] reported that the spe-
et al. [39] include: cific resistance for lower crossflow velocities was greater than
the one obtained in higher crossflow velocities for all yeast cell
When salts do not cause aggregation in the feed, the perme- concentrations tested. In contrast, during the membrane filtra-
ability of the cake layer sharply decreases with the increase tion of monodisperse latex particles, no effect of stirring speed
in electrolyte concentration. was found on the specific resistance values [43].
The permeability of the cake layer sharply decreases with the The compressibility indexes of the cake have been found to
increase in permeate flux because the increased flux results in be different in crossflow and dead-end filtration. Keskinler et al.
a more compressed cake layer. [44] found that non-living yeast cakes formed in the crossflow
The permeability of the cake layer increases with the surface mode are more compressible than cakes formed in dead-end
potential of the particles due to the increase in the inter- filtration. The compressibility index was found to be 1 and
particle repulsion. However, above a certain value of surface 0.39 for the crossflow and dead-end filtration, respectively.
potential, a plateau value for the permeability is reached. Xujiang et al. [49] found similar trends during microfiltration
The permeability of the cake layer passes through a minimum of talc suspensions. By contrast, Mota et al. [50] reported that,
with the increase in the particle size. for spherical particles, the compressibility index (n) both in
dead-end and crossflow filtration were similar basing on the with alginate, a microbial polysaccharide, showed increasing
studies at relatively low crossflow velocity. Tanaka et al. [45] specific resistance with time, indicating a consolidation of the
found lower compressibility index in crossflow filtration than cake layer formed which may be due to infiltration of small
that in dead-end filtration during microfiltration of rod-shaped fractions of the alginates among the alginate aggregates initially
B. subtilis, which are 0.6 and 0.8, respectively. They explained trapped by the microfilter. When both alginate and protein are
these differences as follows. During the crossflow filtration present, the transmission of both components was reduced while
at lower TMP, the cells were arranged by the shear from the the compressibility of the mixed deposit was increased. Thus the
beginning of cell deposition on the membrane surface, thus the rigidity and compressibility may vary substantially depending
cake showed higher specific cake resistance than that in the on the chemical nature of the extracellular components bound
dead-end filtration. While at higher TMP, the cells deposition or soluble in MBR or fermentation broths.
at the initial stage of crossflow filtration in particular tended to Some researchers indicated that particles in the mixed feed
deposit in a manner similar to that in dead-end filtration due to solution determine the flux behavior during the membrane fil-
the high permeate flux; therefore the specific cake resistance tration. Timmer et al. [58] found that the small quantities of
became close to that in the dead-end filtration. This may provide silicates completely determined the flux behavior in the cross-
the reason that the compressibility is lower in crossflow filtration flow microfiltration of -lactoglobulin solutions. Causserand et
than dead-end filtration. Hughes and Field [51] recently showed al. [59] studied the permeability changes in clay cake due to
that increasing shear stress reduced the amount of reversible protein adsorption. A minimum limiting flux was found at the
fouling in yeast filtration but the irreversible component isoelectric point of the clayprotein complex. Interestingly, they
remained constant. The potential for size segregation and lateral found that at higher pH values, the mixture behavior was simi-
transport for yeast cells near the membrane wall has also been lar to the protein, whereas below pH 4.5, the limiting flux was
observed [52]. Foley [53] recently reviewed factors affecting similar to those observed for the filtration of clay suspensions
filter cake properties of microbial suspensions. alone. By optimizing the electrostatic interactions between pro-
For complex fluids such as membrane bioreactors effluent, teins and an adsorptive surface like clay, Causserand et al. [60]
fermentation broths, and natural organic matter, the fouling improved protein fractionation and decreased membrane foul-
interactions of the colloidal component are affected by the poten- ing by the protein, which was attributed to the formation of a
tial for small macromolecules to penetrate and adsorb into the secondary membrane by clay particles on top of the original par-
membrane structure and foulant cake structure. On the other ticles. Hwang et al. also showed that capture of BSA in bed of
hand, colloids or particles can affect the initial deposition of the latex particles can be related by standard capture equation for
macromolecules by adsorbing them on their surfaces or provid- deep-bed filtration. Interesting studies by van Oers et al. showed
ing a secondary layer that entraps aggregates of these macro- how the presence of silica sols can reduce rejection of polyethy-
molecules. Studies to elucidate this phenomenon have been lene glycol (PEG) and dextran by providing a high polarization
carried with yeast and protein mixtures. Davis and colleagues layer (unstirred) zone near the membrane [61]. In contrast, the
[5456] showed that the presence of yeast actually prevented rejection of PEG and dextran increased in the presence of BSA.
fouling of bovin serum albumin (BSA) in microfiltration as the The compressibility of the BSA layer leads to highest rejection
yeast layer on the membrane surface captured the BSA aggre- occurring at the highest pressure of filtration.
gates and prevented them from fouling the internal structure of The impact of large particles on the fouling process is not easy
the membrane. In this case, the cake layer formed by the yeast to gauge. Researchers have indicated that fouling can be reduced
particles can be considered as a prefilter (Fig. 2). They observed by adding suspended solids during UF of organic molecules
higher protein transmission and higher flux in the presence of such as polysaccharides and proteins. Panpanit and Visvanathan
the yeast cake than in its absence. Recent studies by Ye and [62] investigated the role of bentonite addition in the UF for
Chen [57] showed that the critical flux of the mixtures of yeast oil/water emulsions. It was found that the addition of ben-
and BSA showed little change from critical flux measured for tonite up to a certain concentration dramatically decreased the
yeast alone; however, the reversibility of the deposited formed membrane fouling. This was because the reduction of oil/water
by these mixed layer is substantially reduced. Thus the macro- emulsions concentration by bentonite adsorption and the forma-
molecules can serve to bind the particulates together. Results 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
Fig. 2. Cake layer as prefilter. or particulate cakes which form with swollen macromolecular
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
Fig. 3. Composite cake structure. agent, the important role of matrix in resistance was confirmed
by the changes of flux and specific cake resistance [68].
underlayer may disengage spontaneously if the cake build-up is 2.4. Effect of membrane morphology and surface chemistry
sufficient to create high shear stress due to crossflow [63]. on fouling mechanisms
In systems with the microorganisms, the likelihood of dif-
ferent cell wall properties precluded researchers from making Conventional wisdom generally attributes lower fouling to
definitive statements regarding the effects of cell size and shape smooth hydrophilic membranes with high porosity and narrow
on filtration characteristics. In this context, Foley and his co- pore size distribution. This has been supported by extensive work
workers used polymorphic microorganisms to conduct a detailed with various biological fluids, particularly proteins solutions
investigation of the effect of cell size and shape on filtration [10,11,70,71]. Reduction in the macromolecular adsorption with
behavior [48,6467]. The shape of this microorganism, ranging hydrophilic surfaces or by mitigating charge interactions will
from yeast-like to filamentous, could be varied in a controlled reduce the rate of pore closure due to this mechanism. Met-
way by altering its growth conditions. The structure of the cell samuuronen et al. [72] reported that much lower critical fluxes
wall was reasonably constant and independent of the cell shape. were observed for the ultrafiltration of bakers yeast when a
The results clearly showed that the specific cake resistance hydrophobic polysulfone membrane was used as opposed to a
and compressibility of the microbial filter cakes was strongly hydrophilic regenerated cellulose membrane. This phenomenon
related to cell morphology, in particular the mean aspect ratio is more obvious at pH 6 where both membranes have a zeta
of the cells. The potential errors in calculating specific resis- potential of zero. By using matrix-assisted laser desorption ion-
tance and tortuosity is significant in mixed species cakes and ization mass spectrometry (MALDI-MS) for quantitative analy-
the effect of cell shapes and structure in a compressible media sis, Chan et al. [73] studied the membrane fouling by protein
may require better understanding of the associated extracellular mixtures on hydrophilic and hydrophobic 30 kDa molecular
material [50,68]. weight cut-off (MWCO) UF membranes. It was found that, for
Recent work by Ohmori and Glatz [69] and earlier work by the hydrophobic membrane, the deposition exceeded quantities
Hodgson et al. [68] have shown that the filtration properties of corresponding to a monolayer above and below the apparent
microbial suspensions were dependent not only on the cell shape critical flux. When a hydrophilic membrane was employed,
but also on the physical characteristic of the cell and associated coverage in excess of a monolayer was only found above the
extracellular matrix. Ohmori and Glatz [69] found that changes 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-
Fig. 4. Velocity profile during filtration of binary model solution with direct
observation apparatus (500 mg/l alginate50 mg/l bentonite solution; apparent fer in various studies. In the microfiltration of 0.4 wt.% BSA
bulk velocity = 2 mm/s; constant flux of 56 l/m2 h). The background picture solutions, Chen [75] found that the critical flux increased with
shows the fouling layer after 2 h of filtration. 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 The long-term effect of UF membrane pore size on hydraulic
performances has been assessed by He et al. for anaerobic MBR
3.1.1. Physical parameters operated under constant TMP [87]. The smallest MWCO tested
3.1.1.1. Pore size and distribution. The effects of pore size (and (20 kDa) featured the largest permeability lost within the first
distribution of pore size) on membrane fouling are strongly 15 min of filtration when compared to 30, 50 and 70 kDa mem-
related to the feed solution characteristics and in particular branes. However, when operated for extended time (over 100
the particle size distribution. Depending of the pore size and days) with regular hydraulic and chemical cleaning, the largest
the type of biomass filtered, results reported in the literature MWCO membrane (70 kDa) experienced the greater fouling
have shown opposite trends. If particle size is smaller than rate, as 94% of its original permeability was lost, compared to
pore size, pore blocking and/or restriction is expected. It is only 70% performance decrease for the other three membranes.
therefore expected that large pore membranes like MF would As a result, the 30 and 50 kDa membranes provided the best
present higher fouling propensity compared to UF membranes. overall hydraulic performances, indicating the possibility of an
Table 2 reports results obtained in 11 studies during which optimum membrane pore size for a given application and for a
the pore size effects have been assessed by different fouling given filtration time. These results also revealed that the experi-
parameters. It is quite clear from this table that the pore size ment duration is crucial to fully assess the fouling propensity of
alone cannot predict hydraulic performances as no general trend a membrane. Similar trends showing the time dependency for
was observed between these two parameters. The complex and large pore MF with the highest initial fouling for the smaller
changing nature of the biological suspension present in MBR pore and the greater long-term fouling for the larger pore were
systems and the large pore size distribution of the membrane reported for pore size ranging from 1.5 to 5 m operated at con-
generally used in MBR are the main reasons for the unde- stant TMP [90]. While the quest for the highest steady-state
fined general dependency of the flux propensity on pore size permeability is probably desirable, it is important to be aware
[83,84]. Additionally, the duration of the experiment and other that conclusions derived from flux decline data could be some-
operating parameters like crossflow velocity (CFV) and con- times deceptive, as an intrinsically high flux membrane may
stant pressure or constant flux operation have a direct influ- appear to foul more for the same increment of resistance.
ence on the determination of the optimization of the membrane It is expected that smaller pore membranes would reject a
pore size (Table 2). For example, when MF and UF mem- wider range of materials, and the resulting cake layer features a
branes were compared in a similar environment (with a CFV higher resistance compared to large pore membranes. However,
of 0.1 m/s), the MF membrane produced a hydraulic resistance this type of fouling is more reversible and is easily removed dur-
around twice that of the UF membrane. In that same study, the ing the maintenance cleaning than fouling due to internal pore
fouling behaviors of the MF and UF membranes were differ- clogging obtained in larger pore membrane systems. The irre-
ent when operated at higher CFV. This was due to the effect versible fouling, due to the deposition of organic and inorganic
of CFV on critical flux of particulates (Section 3.3.1). Inter- materials onto and into the membrane pores is the main cause
estingly, the dissolved organic carbon (DOC) rejection of both of the poor long-term performances of larger pore size mem-
membranes were similar after 2 h of operation, indicating the branes. However, when testing membranes with pores ranging
creation of a dynamic membrane layer on the MF membrane from 0.4 to 5 m (at constant TMP), Gander et al. observed
[85]. 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
Fig. 11. Proposed method for EPS and SMP extractions and measurements.
Table 4
Concentration of the eEPS components in different MBR systems (units are in mg/gSS by default)
eEPSp eEPSc Other Details References
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 supernatant rather than those filtering 4 g/l of biomass. This
distinct peaks. The analysis of the complex mixtures of eEPS example clearly indicates that the composition and concentration
polymers revealed the presence of 45670 kDa MW proteins, of the organics present in the biomass supernatant (i.e. soluble
and 0.51 kDa MW carbohydrates. The presence of both pro- microbial products (SMP)) have a large impact on membrane
teins and carbohydrates around the biological cells was proposed performance. SMP are defined as soluble cellular components
as a key parameter in the floc formation, and therefore may also that are released during cell lysis, diffuse through the cell mem-
have a significant role in MBR fouling. From this point of view, brane, are lost during synthesis or are excreted for some purpose
the work reported for characterization of eEPS obtained from [187,209]. In MBR systems, they can also be provided from the
CASP and their influence of flocculation, settling and dewater- feed substrate (Fig. 10). It has been now widely accepted that the
ing may also be an interesting parallel for MBR fouling. Recent concepts of soluble EPS and SMP are identical [152,175,187].
reviews [185,205] reporting these issues are valuable tools for During filtration, SMP adsorb on the membrane surface, block
future EPSMBR studies. membrane pores and/or form a gel structure on the membrane
Since the EPS matrix plays a major role in the hydrophobic surface where they provide a possible nutrient source for biofilm
interactions among microbial cells and thus in the floc forma- formation and a hydraulic resistance to permeate flow [152].
tion [185], it was proposed that a decrease in EPS levels may Although the influence of dissolved matter has been studied for
cause floc deterioration. Experimental results obtained during a decade, the concept of SMP fouling in the MBR is relatively
the comparative study of nitrification/denitrification in a MBR new as no report on SMP levels existed for MBRs prior to 2001
tend to confirm this theory [175]. The repercussion of low EPS [83]. In order to reveal the feasibility and relevance of liquid
level, and therefore floc deterioration on membrane fouling may phase analyses on MBR filterability and potentially standardize
be detrimental for the MBR performances. If verified more thor- the method, Rosenberger et al. reported four MBR cases studies
oughly, this would indicate the existence of an optimum EPS based on SMP analysis for membrane fouling [152].
level for which floc structure is maintained without featuring Three methods of separating the water phase from the
high fouling propensity. biomass have been investigated, and the simple filtration through
Many parameters including gas sparging, substrate composi- filter paper was found to be the most effective technique over
tion [171], loading rate [206,207] affect EPS characteristics in centrifugation and sedimentation [210]. Although these authors
the MBR, but SRT probably remains the most significant of them used a large pore filter paper (12 m), it is suggested in this
[208]. A clear decrease of EPS levels was observed for extended review to filter the solution with, at least, a 1.2 m filter in order
SRT, but this reduction became negligible for SRT greater than to remove colloids (Fig. 11). Similarly to eEPS, SMP solution
30 days [165]. However, Lee et al. [181] observed an increase is then characterized with its relative amount of protein and
in protein concentration (along with stable carbohydrate levels) carbohydrate [210], with its TOC level [200] or more rarely
when SRT was increased. Further comments on the role of SRT with SUVA measurement [211]. Examples of SMPp and SMPc
are given in Section 3.3.2. reported in the literature are given in Table 5.
HPSEC analysis has also been conducted on SMP solutions
3.2.6. Soluble microbial products (SMP) (Fig. 12). Not surprisingly, the molecular weight distribution
In an attempt to protect the membrane from direct contact of the organics present in MBR supernatant was found to be
with MLSS, a dual compartment MBR (bioreactor coupled with significantly different for reactors operated under various con-
settling tank in which membrane filters biomass supernatant) ditions [158]. However, the SMP solution fingerprint was largely
has been built in Singapore [207]. In this set-up, higher fil- unchanged for weekly measurement from the same reactor, indi-
tration resistance was observed from the membranes filtering cating no significant change in SMP characteristics when the
Table 5
Concentration of the SMP components (in mg/l)
SMPp SMPc Other Operating conditions References
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.
biomass is acclimatized to given operating conditions. When [208]. However, in two separate studies, analyses of the foul-
compared to EPS molecular weight distribution, the SMP solu- ing layer have revealed a higher concentration of carbohydrate
tion featured generally larger macromolecules [165]. and lower concentration of proteins compared to their levels in
Comparison between acclimatized sludges obtained from the activated sludge [86,218]. This further confirms the greater
MBR and CASP pilot plants revealed similar levels in terms distribution of SMPc in the fouling layer compared to that of
of eEPSp, eEPSc and eEPShumic [180]. The presence of the SMPp. With a smaller MW, humic substances contained in the
membrane in the MBR process does not seem to affect the liquid phase are not retained by the membrane, and therefore
content of eEPS within the flocs. However, SMPp, SMPc and may not significantly participate to MBR fouling [217].
SMPhumic levels were significantly greater for the MBR sludge, As expected, many operating parameters affect SMP levels
presumably due to the retention of large macromolecules by the in MBRs. As for eEPS, SMP levels decreased with increasing
membrane. Critical flux tests carried out under the same condi- SRT [165]. For SRT ranging from 4 to 22 days, SMPp and SMPc
tions for both MBR and CASP sludges revealed the higher foul- levels were reduced by factors of 3 and 6, respectively [213]. In
ing propensity of MBR sludge over CASP (critical fluxes were their long-term study, Rosenberger et al. identified temperature
around 1015 and 3243 l/m2 h, respectively). Since the mea- and stress to the microorganisms (and at a lower degree, SRT)
sured levels of EPS was unchanged, only the SMP components to be the main parameters affecting SMPc [158].
can be accounted for the higher membrane fouling observed for In order to obtain better control of the environmental con-
MBR sludge [180]. During this study, Cabassud and co-workers ditions, many research studies are based on the use of syn-
observed significant biological activity in the MBR supernatant, thetic/analogue solutions, which attempt to model real wastew-
indicating the presence of free bacteria (presumably submicron aters. These solutions are sometimes very basic (mainly com-
colloidal size), which could also be another cause of mem- posed of glucose) and therefore are very easily biodegradable.
brane fouling. Direct linear relationships between loss of MBR As a result, it is expected that SMP levels in such systems are
hydraulic performances and SMP concentration has been also lower than in real systems. Since it may be assumed that there are
reported for an anaerobic MBR [171] and has been mathemat- almost no substrate residuals from glucose in the supernatant,
ically modeled [214]. Different mechanisms for the interaction the less biodegradable SMP induced by cell lysis or cell release
between the macromolecules present in the supernatant and the would account for most of the SMP measured in synthetically fed
membrane surface have also been proposed recently [158]. The MBRs. This could explain the lower influence of SMP compared
creation of the fouling layer on the membrane surface would to those of eEPS reported in some MBR studies. When using syn-
act as a secondary membrane, increasing the retention and/or thetic substrate, Cho et al. [197] concluded that the membrane
the adsorption of macromolecules. The formation of a biofilm fouling was affected more by the bound EPS of activated sludge
could also lead to the degradation of the macromolecules as floc rather than the dissolved organic matter. SUVA measure-
the permeate flows through the membrane. Finally, interaction ment carried out from supernatant of MBR fed with synthetic
between the macromolecules and other solutes (humics, divalent solution confirmed the presence of a portion of larger, more aro-
cations) within the membrane pores may be responsible for the matic, more hydrophobic and double-bond-rich organics, which
reduction of the membrane pore size over time. originated from the decayed biomass rather than the feed [211].
In an attempt to define the biomass fraction with the highest Another important study [219], also based on synthetic wastew-
fouling potential, Lesjean et al. [150] conducted a methodi- ater, revealed that soluble organics alone cannot predict MBR
cal comparison between permeate and supernatant solutions. fouling. By comparing filterabilities of attached and suspended
Assuming that the materials observed in the biological super- growth microorganisms, Lee and co-workers observed the rate
natant and not in the permeate solution are responsible for MBR of membrane fouling of the attached growth system (MLSS
fouling, this group clearly revealed the higher concentration of 0.1 g/l and attached biomass of 2 g/l) to be about seven times
carbohydrates, proteins and organic colloids in the MBR super- higher than that of suspended growth MBR (MLSS of 3 g/l).
natant compared to those in the permeate. These findings con- With similar soluble fraction characteristics in both reactors,
firmed similar results previously reported [30,210]. Since, direct the filtration discrepancy was explained by the formation of a
relationships between the carbohydrate level in SMP solution protective dynamic membrane created by suspended solids. The
with fouling rate [150], filtration index and CST [213,215,216], results of Ng et al. [207] reported earlier, with more fouling
critical flux tests [102], and specific flux [152] have been clearly from supernatant that mixed liquor, can also be explained by this
described, this reveals the SMPc as the major foulant indicator mechanism.
in MBR systems. However, the nature and fouling propensity Another group of organic materials has been recently
of SMPc were observed to change during the study of unsteady introduced by Wang et al. [220]. The biopolymer clusters
MBR operation [217]. In this specific study, it was not possi- (BPC) have been defined as non-filterable material issued from
ble to correlate SMPc to fouling. So far, the effect of the protein the affinity clustering of the free EPS and SMP present in the
fraction contained in the SMP solution on MBR fouling has been sludge cake deposited on the membrane surface. Although
more rarely reported. Since a significant amount of proteins is BPC is expected to accumulate on the pore of the sludge cake,
retained by the membrane (from 15% [210] to 90% [217]), it this material can be readily separated from the fouling cake by
is expected that this plays a role in MBR fouling. This was simple stirring. This work highlights the recent interest in the
recently confirmed by the value of specific resistance increasing polymeric characterization of the fouling layer [172,221]. For
by a factor of 10 as the SMPp increased from 30 to 100 mg/l this purpose, confocal laser scanning microscopy can be used
to precisely locate different EPS compounds on the membrane ies, the limits of the aeration were demonstrated through its effect
surface [172,176,222,223]. on the netflux-ratio (netflux over instantaneous flux calculated
for operation with membrane relaxation or backwashing). In this
3.3. Operating conditions case, aeration intensity could not further improve hydraulic per-
formances below the critical netflux-ratio of 0.85. Above this
3.3.1. Aeration, crossow velocity value, the aeration rate was able to limit, to a certain extend,
Controlling fouling in submerged membrane systems the formation of severe fouling [239]. This study revealed that,
remains more challenging than in pumped crossflow or dead-end for specific conditions, the filtration mode has more effect on
rigs, in which the feed-liquid can be more accurately managed. MBR fouling than the changes in aeration rates. Intense aera-
Since the origin of the submerged MBR, bubbling has been tion rate may also damage the floc structure reducing their size,
defined as the strategy of choice to induce flow circulation and and releasing EPS in the bioreactor [174,240]. These phenomena
shear stress on the membrane surface. Aeration used in MBR have been similarly described in the sidestream MBR configura-
systems has three major roles: providing oxygen to the biomass, tion in which the circulation pump is responsible for the break up
maintaining the activated sludge in suspension and mitigating of bacterial flocs [241,242]. However, in a small crossflow cell,
fouling by constant scouring of the membrane surface [224]. The fouling was found to decrease linearly with increasing CFV (up
use of gas bubbling to enhance membrane processes, and MBRs to 4.5 m/s), and no CFV optimum was observed [243]. Detailed
in particular, has been thoroughly investigated and reviewed study of the various calculated hydraulic resistances revealed
[106]. While fundamental studies and mathematical models have that CFV values of 2 and 3 m/s were sufficient to prevent the
been applied to well-defined membrane configurations (such as formation of reversible fouling in UF (30 kDa) and MF (0.3 m)
tubular [225,226] and flat sheet [227229]), the effect of bub- systems, respectively. Finally, it was shown that high CFV was
bles on submerged hollow fiber modules is still being assessed. more effective in reducing fouling in the MF rather than in the
More recently, the uneven distribution of the aeration turbulent UFMBR system. This was confirmed by analysis of the mass,
shear intensity has been taken into account in the development thickness and density of the fouling layer deposited in/on the
of a mathematical model [230]. Theoretical analysis becomes membrane under different operating conditions. This may be
even more problematical when the complex nature of biomass due to the effect of CFV on critical flux of particulates. At a
mixture (non-Newtonian fluid containing solutes, colloids and low CFV of 0.1 m/s, the UF membrane fouled less, being less
particulates) present in MBRs is taken into account. However, susceptible to the particle deposition, whereas at a high CFV
general anti-fouling phenomena due to aeration occurring in of 3.5 m/s, the majority of particles would not deposit (raised
MBRs can be described. critical flux) on either membrane. However in current MBRs
Basically, the bubbles flowing near to the membrane sur- generation, the CFV is relatively low which could favor the use
face induce local shear transients and liquid flow fluctuations, of tighter (UF) membranes.
increasing back transport phenomenon. The tangential shear at Determination of the CFV induced by aeration of the mem-
the membrane surface prevents large particle deposition on the brane surface can be difficult to assess and techniques such
membrane surface. However, the effect of tangential shear is a as electromagnetic flow velocity meter [244], particle image
function of particle diameter, with lower shear induced diffu- velocimetry [232], constant temperature anemometry [245,246],
sion and lateral migration velocity for smaller particles, leading have be used for liquid velocity estimation in submerged MBR
to more severe membrane fouling by fine materials [231]. Aer- reactors. Based on the observed CFV in tap water in the riser
ation also affects MBR performance by causing fiber lateral section (CFVtp ) of a internal loop-airlift MBR system, Liu et al.
movement (or sway) in hollow fiber configurations [121]. The set up a modified model for calculating the CFV of the aerated
effect of bubbling can help to overcome issues related to high activated sludge (CFVas ) over the membrane surface [237]:
packing density in hollow fiber bundles. However, it is still a
challenging task for MBR designers to achieve effective aeration CFVas = 1.406 CFV1.226
tp 0.147 (3)
throughout the population of fibers in a bundle [232]. All these
effects, described in more detail elsewhere [104,106,233235], where is the viscosity of the MLSS, and CFVtp can be esti-
contribute to a significant reduction in fouling propensity. A mated from equation given in Liu et al.s earlier publication
novel explanation for the influence of aeration on MBR foul- [247].
ing has been proposed by Ji and Zhou [174]. According to their
results, aeration rate directly controls the quantity and composi- 3.3.2. Solid retention time (SRT)
tion of the polymeric compounds (EPS) in the biological flocs, SRT (and consequently the F/M ratio), which ultimately con-
and ultimately the ratio of protein/carbohydrate deposited on the trols biomass characteristics, is probably the most important
membrane surface. However, this mechanism cannot explain the operating parameter impacting on fouling propensity in MBRs.
effects of bubble-induced fouling control observed with model Operating an MBR at higher SRT leads inevitably to increase of
feeds [121]. MLSS concentration, but this in itself may not necessary lead to
An optimum aeration rate, beyond which a further increase greater fouling (Section 3.2.3) [248].
has no significant effect on fouling suppression, was originally Extremely low SRTs (down to 2 days) have been tested
observed by Ueda in 1997 [236], and has been verified in many to assess fouling propensity [249]. Not surprisingly, fouling
occasions since [84,237,238]. During MBR optimization stud- rate increased nearly 10 times when SRT was lowered from
10 to 2 days (corresponding to F/M ratio from to 0.5 to for very long SRT. However, the difficulty related to properly
2.4 gCOD/gMLVSS/day and MLSS of 7.86.9 g/l). There is no acclimatize an MBR (pilot) plant to different SRTs and conduct
reason (other than purely research-based work) to run MBRs a fair comparison does not allow the determination of an opti-
at such extreme conditions, and, as a general rule, F/M ratio is mum SRT value. This could also explain the discrepancies in the
recommended to be maintained below 0.5. Other characteris- SRT effects reported in the literature. Criteria such as designed
tics of performance at SRT as low as 0.25 day are discussed in rate of sludge and MLSS concentration recommended by the
[250]. The reasons suggested for the increased fouling rate at membrane supplier is more prone to define the working SRT.
very low SRT include the increased levels of production of EPS. This point is further discussed in Section 4.2.2.
It should be noted that an increased F/M ratio could occur during
transients in unsteady operation (Section 3.3.3). 3.3.3. Unsteady state operation
At the other end of the spectrum, the temptation to run MBRs Unsteady state such as variations in operating conditions
at extended SRT is great, considering the advantages of this pro- (flow input/HRT and organic load) and shifts in oxygen supply
cess over CASP. Indeed the early MBRs were typically run at have also been defined as additional factors leading to changes
very long SRTs to minimize excess sludge. Studies reporting in MBR fouling propensity. In real-world applications, such
operation at infinite SRT are generally bench scale, use syn- unsteady state conditions could occur regularly. In an experiment
thetic feed (or very finely prefiltered sewage) [212,251254] and carried out with a large pilot-scale MBR, the effects of unstable
therefore do not take into consideration the accumulation of inert flow input and unintentional sludge wastage have been assessed
material in the tank. The progressive accumulation in the MBR [217]. Although the level of polysaccharides in the filtrate varied
tank of non-biodegradable materials (like hair and lint), which in a chaotic manner, the concentration of this specific compound
are not completely removed by the MBR pre-treatment pro- increased before and after each sludge withdrawal. While the
cesses, undeniably leads to clogging of the membrane module increase after wastage was due to the sudden stress experienced
[255]. The increase in MLSS concentration related to extended by cells, increase before sludge withdrawal was explained by the
SRT could also result in higher fouling propensity (see Section increasingly high MLSS concentration and the resulting low DO
3.2.3) even with the aeration raised significantly. Previous exper- level in the bioreactor. It was concluded that unsteady operation
iments revealed an increase of MLSS levels from 7 to 18 g/l and changed the nature and/or structure (and fouling propensity) of
a decrease of F/M ratio from 0.15 to 0.05 kgCOD/kgMLSS/day the polysaccharide rather than the overall EPS formation, and
when the SRT was increased from 30 to 100 days. Even after therefore could worsen the fouling propensity. These findings
increasing the aeration rate from 15 to 25 l/min, fouling was confirmed results previously reported on the effects of transient
nearly twice as great for the longer SRT conditions [155]. In conditions in feeding patterns. The addition of a spike of acetate
this scenario, the increased shear provided to control fouling in the feed water significantly decreased the filterability of the
could breakup biofloc as well as causing cell lysis. Moreover, biomass in an MBR; this was due to the rise in SMP levels
the increase in aeration intensity to keep the high MLSS levels resulting from the feed spike [256].
in suspension and properly oxygenated may not be a sustainable The effects of starvation conditions on the biological sus-
option for the treatment process. During a 300-day operation of pension have been assessed by incorporating different substrate
a pilot-scale MBR without wastage (infinite SRT), the MLVSS impulses in batch tests [257]. Exogenous phases were followed
increased steadily from 3 to 15 g/l and both removal efficiency by starvation periods, both characterized by the So/Xo ratio
and membrane performances remained constant. At infinite SRT, (Eq. (4)). For high So/Xo, multiplication of bacteria cells was
most of the substrate is consumed to ensure the maintenance observed, while compound storage, characterized by decrease
needs and the synthesis of storage products. The very low appar- of MLVSS and the absence of SMPp production and bacteria
ent net biomass generation observed can also explain the low lysis, were obtained at low So/Xo ratio. The low F/M conditions
fouling propensity observed for high SRT operation in this study generally used in MBRs are theoretically close to what would
[253]. These two studies show that extended-SRT-operation does be considered as starvation conditions. Although the influence
necessary offer lower fouling; other operating conditions such of these operating conditions on MBR fouling have not been
as flux and aeration rates would also have a major influence on reported, the lower amount of SMPp produced may lead to less
fouling propensity. The other difficulty with very high SRT is severe fouling propensity:
the raised viscosity that could attenuate the effect of bubbling.
So F
The effects of SRT on biological parameters like MLSS, SMP, = HRT (4)
eEPS concentrations, described in Section 3.2, also reveal the Xo M
major impact of this operating parameter on MBR fouling. As with So, the feed substrate concentrate and Xo, the MLVSS
a result, selection of the SRT must be considered very carefully concentration.
in order to optimize MBR operation (see Section 4.2.2). Some The start-up phase can also be considered as unsteady oper-
studies reported the DOC of the supernatant to be independent ation and data collected before biomass stabilization (including
of SRT [252]. The lower fouling generally observed at extended the period necessary to reach acclimatization) may become
SRT is partially explained by the lower organic carbon concen- relevant in the design of MBRs. Cho et al. [197] reported
tration in eEPS rather than in SMP. Overall, it is likely that there temporal changes of the bound EPS levels when the MBR
is an optimal SRT, between the high fouling tendency of very was acclimated to three different SRTs (8, 20 and 80 days).
low SRT operation and the high viscosity suspension prevalent As expected (considering the general trends described in
Section 3.2.5), the concentration of eEPS was lower for the about 10 l/m2 h which is less than normal constant flux MBR
longer SRT (8326 mgTOC/gSS for SRT of 8 up to 80 days, operation. It is important to note that in phase 3, two factors
respectively). More interestingly, an initial latent phase was are at work. Firstly, the lowered flow slows down the convec-
observed for which eEPS concentration did not vary signifi- tion of foulant; it becomes self-limiting. The other factor is that
cantly. However, eEPS levels increased exponentially after 40 once the flux is low, the fouling resistance is high, relative to
days of operation at 8-day-SRT, and after 70 days when the the membrane resistance. To see significant further decline (say
MBR was operated with an SRT of 20 days. No change in eEPS by a further 50%) requires the fouling resistance to double. It
was observed during the 80 days of operation at 80-day-SRT. becomes increasingly difficult to detect fouling trends by simply
In another MBR set-up operated at infinite SRT, no significant inspecting the flux decline profile.
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 3.4.2. Constant ux operation
meantime [258]. After a latent phase of 30 days, MLSS and SMP With the constant flux approach, the convection of foulant
levels started to significantly increase and stabilized by reaching does not diminish and fouling phenomena self-accelerates and
a plateau after 140 days of operation at infinite SRT (operated for can eventually create a sharp increase of TMP. With fouling rate,
210 days). In this example, eEPS increased continuously from and therefore cleaning frequency, increasing with flux, operation
day 1 to also reach steady-state on day 140 [251]. Nagaoka and conditions favors the MBR to be run at modest fluxes to limit
Nemoto [198] observed a rise of MLSS concentration from 4 fouling severity (Section 4.2.2). As a result, numerous studies
to 14 g/l over 100 days (SRT value not given) along with a rel- have reported the fouling behavior for long-term MBR filtration
atively constant increase in eEPS (from 50 to 250 mg TOC/l). carried out at sub-critical flux. However, these long-term exper-
From these examples and the relationship between eEPS-SMP iments have revealed noticeable fouling for MBRs operated at
and fouling propensity defined earlier, further research on the sub-critical flux. Since its first reference to MBRs in 2001 [28],
exact impact of unsteady states on MBR fouling is required to fouling behavior over time is generally characterized by a two-
implement more sustainable MBR operation. At this point in step pattern. During the first period, a very small TMP rise was
time, the evidence points to increased membrane fouling during observed. For trials carried out over extended time periods, a
unsteady state (particularly when F/M is increasing). noticeable change in the rate of TMP increase then arises after
some critical time period (Fig. 13). Pollice et al. [32] reviewed
3.4. Fouling mechanisms in MBRs the phenomena and two parameters were introduced as indica-
tors for operation under sub-critical conditions: the critical time
3.4.1. Constant TMP operation over which the prolonged first step is maintained (tcrit ) and the
The current trend in MBR design is to operate at constant flux, fouling rate (dTMP/dt) during that step. Table 6 reports tcrit and
and as a result, very few recent studies report the operation of dTMP/dt for recent trials and reveals the long periods of filtra-
MBR at constant TMP. In the MBR, like other membrane filtra- tion (up to 1200 h) for which fouling rate can be maintained at
tion processes at constant TMP, a rapid flux decline is expected to very low values (down to 2 104 kPa/h). The fouling rates for
occur during the initial stages of the filtration. The rate of fouling the high TMP-rise-period have also been reported previously
then decreases before reaching a plateau. Bae and Tak recently [148]. Prior to these two filtration-steps generally described
summarized the hypothetical three-phase-process-mechanisms in the literature, a conditioning period has also been observed
for initial cake layer formation occurring in MBR [143]. They [86]. This conditioning period (from now called stage 1) has
filtered MBR mixed liquor samples at 100 kPa over periods of not been observed or described as such until recently, but may
up to 5 h with a range of UF membranes. According to these be a key aspect of fouling creation in MBRs. The dynamics of
authors, the main parameter affecting the initial fouling (phase 1) the biomass detachment from the membrane in relation to the
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 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 considers macroscopic redistribution of flux, the pore loss
the separation surface and contribute to stage 2. model focuses on microscopic scale. In MBR systems, it is
expected that both mechanisms occur simultaneously.
3.4.2.2. Stage 2slow (steady) fouling. Even though MBRs (iii) The critical suction pressure model. Using a fine colloid,
are operated below the critical flux for the biomass, biofloc may filtered in dead-end mode, onto an immersed hollow fiber,
randomly land (see above) and contribute to the second foul- gradual TMP rise followed by a rapid increase in TMP was
ing stage. After stage 1, the membrane surface is expected to observed. Both autopsy and modeling suggested a critical
be mostly covered by SMP, leading to the higher attachment suction pressure at which coagulation occurs at the base
propensity of biomass particles and colloids. Because of the low of the cake [266]. The very thin dense layer observed next
critical flux determined for SMP species, further adsorption and to the membrane confirmed the rapid increase in resistance
deposition of organics on the membrane surface may also occur leading to the TMP jump. Although this model was obtained
during stage 2. Since adsorption may take place not only at the with dead-end rather than crossflow operation, there is no
membrane pores but also on the whole surface, biological flocs reason why this mechanism could not apply to sidestream
may initiate cake formation without directly affecting the perme- or submerged MBRs. A requirement for that model is that
ability in this stage. Over time, this phenomenon would worsen. fouling continues to occur over time until the critical suction
The rate of EPS deposition, and resulting TMP rise, is expected pressure is reached, and that the deposit compound(s) have
to increase when the operating flux is higher, leading to a shorter the potential to coalesce or collapse. Biofilms and deposit
stage 2 operation (Table 6). The fouling mechanisms described layers in MBRs are likely to have this tendency.
above would prevail even with a good hydrodynamic environ- (iv) Percolation theory. According to percolation theory, the
ment that provides adequate surface shear over the membrane porosity of the fouling layer gradually reduces due to the
surface. However as maldistributions of flow, shear or flux are continuous filtration and material deposition within the
generally expected in MBRs, irregular fouling patterns can be deposit layer. At a critical condition, the fouling cake loses
anticipated. connectivity and resistance, and TMP, increase rapidly. This
model has been proposed for MBRs [34], but the model indi-
3.4.2.3. Stage 3TMP jump. With regions or pores of the cates a very rapid change (within minutes), which has not
membrane more fouled than others, flux is expected to sig- been observed in practice. However, it is plausible that the
nificantly decrease in those specific locations. As a result, the percolation theory approach, combined with the inhomo-
overall permeate productivity redistributes to the less fouled geneous fouling (area loss) model, could satisfy the more
membrane areas or pores, for which local flux increases (see gradual kinetics of the typical TMP transient. Similarly,
Section 2), exceeding a critical flux (defined as sustainable flux fractal theory was successfully applied to describe cake
in Section 4.2.2). These phenomena have a self-accelerating microstructure and properties and to explain the cake com-
nature and severe fouling, characterized by an exponential pression observed during MBR operation [267].
TMP increase, is generally obtained if the filtration is main- (v) The inhomogeneous ber bundle model. Another manifes-
tained. The sudden rise in TMP or jump is a consequence tation of the TMP transient has been observed for model
of constant flux operation and several mechanisms can be pos- fiber bundles where the flow from individual fibers was
tulated for the rapid increase in TMP at a given condition monitored [118]. The bundle was operated under suction
[86]: at constant permeate flow, giving constant average flux, and
initially this was evenly distributed amongst the fibers. How-
(i) The inhomogeneous fouling (area loss) model. This model ever over time, the flows became less evenly distributed so
was proposed to explain the observed TMP profiles in nom- that the standard deviation of the fluxes of individual fibers
inally sub-critical filtration of upflow anaerobic sludge [25]. started to increase from the initial range of 0.10.15 up to
The TMP jump appeared to coincide with a measured loss 0.4 l/m2 h. Consequently, the TMP rose to maintain the aver-
of local permeability at different positions along the mem- age flux across the fiber bundle, mirroring the increase in
brane, due to slow fouling by EPS. It was argued that the the fluxes standard deviation. At some point both TMP and
flux redistribution (to maintain the constant average flux) standard deviation showed a rapid rise. This is believed to
resulted in regions of supra-critical flux and consequently be due to flow maldistribution within the bundle leading
in rapid fouling and TMP rise. to local blockages between fibers and membrane fouling. It
(ii) The inhomogeneous fouling (pore loss) model. Similar TMP was possible to obtain more steadily TMP and standard devi-
transients have been observed for the crossflow MF of a ation profiles when the flow regime around the fibers was
model biopolymer (alginate) [17]. These trends revealed more vigorous (higher liquid and/or air intensity). Although
that the TMP transient can occur with relatively simple this trend was observed for a small model bundle, the phe-
feeds. The data obtained have been explained by a model that nomena are likely to occur in larger bundles.
involves flux redistribution among open pores, allowing for
the pore size distribution. Local pore velocities eventually The mechanisms (i)(v) listed above are all self-accelerating
exceed the critical flux of alginate aggregates that rapidly and this is a feature of stage 3 fouling. It is probable that more
block the pores. This idea was also the basis of the model than one of these mechanisms apply simultaneously when an
proposed by Ognier et al. [31]. While the area loss model MBR reaches the TMP jump condition.
4. Mitigation of MBR fouling ent. The fouling removal efficiency of this method can be fur-
ther increased when air scouring is applied during relaxation
4.1. Removal of fouling [149,274]. Detailed studies of the TMP behavior during this
type of operation revealed that although the fouling rate is gen-
4.1.1. Physical cleaning erally higher than for continuous filtration, membrane relaxation
Physical cleaning techniques for MBRs include mainly mem- allows filtration to be maintained for longer period of times
brane relaxation (where filtration is paused) and membrane before the need for cleaning [207]. Although some have reported
backwashing (where permeate is pumped in the reverse direction that this type of operation may not be economically feasible for
through the membrane). These techniques have been incorpo- large-scale MBRs [149], further cost and productivity analysis
rated in most MBR designs as standard operating strategies to are probably required to compare this method against backwash-
limit fouling; although vigorous backwashing is not an option ing. Recent studies assessing alternative strategies for fouling
for flat plate submerged membranes. mitigation tend to combine intermittent operation with frequent
Backwashing (also called backflushing) has been found to backwashing for optimum results [137,275].
successfully remove most of the reversible fouling due to pore
blocking, transport it back into the bioreactor, and partially dis- 4.1.2. Chemical cleaning
lodge loosely attached sludge cake from the membrane surface. It is expected that membrane relaxation and backwashing
In some cases, clogging near the membrane surface may also be effectiveness tend to decrease with operation time as more irre-
partially loosened or removed by backwashing. The efficiency of versible fouling accumulates on the membrane surface. There-
backwashing has been studied in detail [268270]. Key parame- fore, in addition to the physical cleaning strategies, differ-
ters in the design of backwashing are its frequency, duration, the ent types/intensities of chemical cleaning may also be recom-
ratio between those two parameters and its intensity. For exam- mended. They include:
ple, less frequent, but longer backwashing (600 s filtration/45 s
backwashing) was found to be more efficient than more fre- Chemically enhanced backwash (on a daily basis),
quent backwashing (200 s filtration/15 s backwashing) [170]. In Maintenance cleaning with higher chemical concentration
another study based on factorial design, suction time (between (weekly), and
8 and 16 min) was found to have more effect on fouling removal Intensive (or recovery) chemical cleaning (once or twice a
than both the aeration intensity (0.30.9 m3 /m2 h) and the back- year).
wash time (2545 s) [239]. Although more fouling is expected
to be removed when backwashing duration and frequency are Maintenance cleaning is used to maintain design permeability
increased, optimization of backwashing is required in regard to and helps to reduce the frequency of intense cleaning. Intensive
energy and permeate consumptions. This was achieved by the cleaning is generally carried out when further filtration is no
design of a generic control system which automatically opti- longer sustainable because of an elevated TMP. Each of the four
mized the duration of the backwash according to the monitored main MBR suppliers (Kubota, Memcor, Mitsubishi and Zenon)
value of TMP [271]. proposes their own chemical cleaning recipes, which differ
This anti-fouling operation obviously affects operating costs mainly in terms of concentration and methods (Table 7). Under
as energy is required to achieve a pressure suitable for flow rever- normal conditions, the prevalent cleaning agents remain sodium
sion. Moreover, between 5 and 30% of the produced permeate hypochlorite (for organic foulants) and citric acid (for inorgan-
is used in the process. Comparison between submerged hollow ics). Sodium hypochloride hydrolyzes the organic molecules,
fiber and flat sheet MBR revealed the slightly higher overall and therefore loosen the particles and biofilm attached to the
flux obtained when operating the membrane constantly at low membrane. The effects of cleaning chemical agents like NaOCl
flux [108]. In this example, flat sheet membranes, which can- on microbial community have been also recently studied for
not be backwashed, were operated constantly with flux ranging modeled MBR processes [276]. It is also common for MBR
between 20 and 27 l/m2 h. The hollow fiber MBR was operated suppliers to adapt specific protocols for chemical cleanings (i.e.
at higher flux (2333 l/m2 h) but with 25% of the permeate prod- chemical concentrations and cleaning frequencies) for individ-
uct being recycled for backwashing (45 s of backwashing after ual facilities [115,179,255]. It also has been mentioned that the
every 600 s of operation). level of pollutants (measured as TOC) in the permeate rises just
Air can also be used as the backflushing medium [272]. after the chemical cleaning episodes [115]. This is important for
Although improving the flux by nearly 400% (compared to con- MBRs used in reclamation process trains (i.e. upstream of RO
tinuous operation), 15 min of air backwash was required every for example). So far, no systematic studies on cleaning agents
15 min of filtration to obtain this result [273]. However, air back- or procedures have been published [277]. This is probably due
washing is an efficient method for flux recovery, it may also to the site-specific nature of the MBR fouling.
present potential issues of membrane breakage and rewetting. Maintenance cleaning, taking up to 30 min for a complete
Membrane relaxation (or non-continuous operation of the cycle, is normally carried out every 37 days at a moderate
membrane) significantly improves membrane productivity. reagent concentration of 0.01 wt.% NaOCl. Recovery cleaning
Under relaxation, back transport of foulants is naturally employs rather higher reagent concentrations of 0.20.5 wt.%
enhanced as non-irreversibly attached foulants can diffuse away NaOCl coupled with 0.20.3 wt.% citric acid or 0.51 wt.%
from the membrane surface through the concentration gradi- oxalic acid (Table 7).
Table 7
Intensive chemical cleaning protocols for four MBR suppliersa (from [255])
Type Chemicals Concentration (%) Protocols
NaOCl 0.3
Mitsubishi CIL Backflow through membrane (2 h) + soaking (2 h)
Citric acid 0.2
NaOCl 0.2
Zenon CIP Backpulse and recirculate
Citric acid 0.20.3
NaOCl 0.01
Memcor CIP Recirculate through lumens, mixed liquors and in-tank air manifolds
Citric acid 0.2
NaOCl 0.5
Kubota CIL Backflow and soaking (2 h)
Oxalic acid 1
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 flux decline was obtained with the TiO2 -membranes compared
layers in MBRs has also been carried out [96]. The sonifica- to that of unmodified membranes.
tion cleaning process is based on the breakdown of the fouling As it was possible to add a larger amount of TiO2 parti-
cake into smaller fragments. Although sonification can success- cles on as a precoat to a membrane, this filter showed greater
fully remove the cake from the membrane surface, this cleaning fouling mitigation compared to that of the TiO2 -entrapped-
method was not effective on all types of fouling due to pore membrane. Similarly, when MBR membranes were precoated
blocking and may even worsen this type of fouling. A combi- with ferric hydroxide flocs and compared to an unmodified
nation of sonification with backwashing and chemical cleaning MBR, both effluent quality and productivity were found to
appeared to achieve almost complete flux recovery [278]. More increase [280]. This phenomenon was explained by the adsorp-
details of the cleaning mechanisms are available in [278]. How- tion of soluble organics on ferric hydroxide flocs, limiting the
ever, sonification would be difficult to apply at a large-scale due direct contact between the organics and the membrane. Finally,
to the focused nature of the sonic energy. fouling phenomena have been used to investigate the creation
of self-forming dynamic membrane coupled bioreactors [281].
4.2. Limitation of fouling By using coarse pore-sized substrates and allowing cake and
gel layers to deposit on the surface, a self-forming membrane
It may also be possible to prevent fouling before its occur- developed with a high flux and good removal efficiencies. How-
rence by (1) improving the anti-fouling properties of the mem- ever, because of the nature of the filtration barrier, the effluent
brane, (2) operating the MBR under specific non-or-little- quality cannot be guaranteed, and this is of concern in many
fouling conditions and/or (3) pre-treating the biomass suspen- applications.
sion to limit its fouling propensity.
4.2.2. Optimization of operating conditions
4.2.1. Optimization of membrane characteristics 4.2.2.1. Aeration. Since the energy involved in providing aer-
In MBRs, chemical modifications of the membrane surface ation to the membrane remains a significant cost factor in MBR
have been shown to efficiently improve anti-fouling proper- design, efforts have been focused on optimization of air flow-
ties. As mentioned above (Section 3.1.2), more severe foul- rate. The specific design of airflow patterns and location of
ing is expected when hydrophobic membranes are used in the aerators have also been defined as crucial parameters in foul-
MBR, and efforts have been focused on increasing membrane ing mitigation. Recent developments in aeration design carried
hydrophilicity through membrane modification. Recent exam- out by MBR suppliers are often reported in patent format, and
ples for MBRs comprise NH3 and CO2 plasma treatments of involve cyclic aeration systems [282], and improved aerator sys-
polypropylene hollow fibers [128,129]. In both cases, X-ray tems [283,284] for example. A recent study reported a detailed
photoelectron spectroscopy (XPS) and SEM were used to char- comparison of various aeration devices used in tubular mem-
acterize the structural and morphological nature of the modi- branes. The results indicated that complex aeration systems with
fied membrane surface. With the introduction of polar groups multiple orifices injecting air homogeneously in the feed flow
(from oxygen and nitrogen) on the membrane surface, mem- featured the highest performances [285]. As mentioned before,
brane hydrophilicity significantly increased and new membranes the effect of aeration varies from hollow fiber to flat plate mem-
presented better filtration performances and flux recovery than brane configurations. The presence of a bi-chamber (riser and
those of unmodified membranes. In another study, the addition down-comer) in a Kubota MBR plays a significant role in induc-
of TiO2 nanoparticles to the casting solution and a precoat of ing high CFV [244]. In the same study, lower uplift resistance
TiO2 allowed the preparation of two types of TiO2 -immobilized and higher CFV were induced by uniformly distributed fine
UF membrane (entrapped and deposited, respectively), which air bubbles (issued from a porous media with 0.5 mm holes)
were also used in MBR systems [143,279]. As a result, lower compared to performances obtained with large bubbles (from
2 mm hole diffuser) at similar aeration rates. The air/permeate more precisely, the use of air sparging. In a specially designed
ratio (m3 /m3 ) can also be a useful parameter to characterize the module in which air bubbles were confined in close proximity
intensity of aeration required to obtain a given amount of treated to the hollow fiber (rather than diffusing in the reactor), higher
water. Values given by MBR suppliers may vary between 24 and permeability was obtained [296].
50, depending of the membrane configuration (flat sheet versus
hollow fiber) and the MBR tank design (membrane and aerobic 4.2.2.3. Sustainable ux. The energy demand for operation is
zone combined into one tank or not) [115]. Preliminary work a potential weakness for the future development of the MBR
carried out in Singapore on large-scale MBRs revealed these process. It is recognized that the energy usage of MBRs is still
original ratios to be quite conservative, since it was possible higher than conventional activated sludge systems due to the
to decrease them (down to 56% of their original value) with- need to control membrane fouling by different strategies. At
out significant fouling increase [115]. Attempts to increase the the end of the day, MBRs can be economically viable only if it
critical flux in submerged MBR by varying the aeration rates delivers a reasonable flux rate without significant fouling. Since
has been reported [286]. In order to minimize fouling during permeation rate and fouling decrease simultaneously, most MBR
high throughput operation, aeration was increased and returned systems operate at low fluxes to limit rapid and severe membrane
to lower values for the low throughput period. Based on these fouling. The concept of sustainable flux in MBRs can be defined
short-term experiments, it was possible to use this technique to as the flux for which the TMP increases gradually at an accept-
minimize energy consumption. However, a recent study from able rate, such that chemical cleaning is not necessary [207]. The
Choi et al. [88] carried out with a crossflow MBR device, indi- rate of TMP increase and the period of filtration before chemi-
cates the tangential shear to have no effect on flux decline when cal cleaning is required are left to the operators discretion, and
pseudo steady-state is reached. In other words, increasing CFV therefore a more detailed definition of sustainable flux cannot
does not decrease fouling intensity when the deposition layer be possible. While critical flux was mainly determined during
starts to govern the permeate flux behavior. In the absence of short-term experiments, sustainable flux can only be assessed
CFV, flux decline was predominantly caused by reversible foul- through longer filtration periods. However, sustainable flux can
ing, while slightly higher irreversible fouling was detected when also be defined as sub-critical flux by default. In such a system,
CFV was applied [88]. not only the flux value is of importance but also the strategies
The intermittent operation of aeration has also been reported used to maintain this given flux.
for (de)nitrification MBR systems [198,287]. In this uncommon
scenario of single tank MBR used for both anoxic and aerobic 4.2.3. Modication of biomass characteristics
biological degradation, filtration is carried out during the aerobic 4.2.3.1. Coagulant/occulent. Ferric chloride and aluminum
phase to take advantage of the anti-fouling properties of the air sulfate (alum) are two types of coagulant commonly used for
scouring. While some authors testing intermittent aeration do not water and wastewater treatments. Both have been added to
recommend this type of operation as severe fouling was observed reduce significantly membrane fouling in MBRs. Once dis-
as soon air sparging ceases [170,238], others have reported that solved in water, alum forms hydroxide precipitates which adsorb
efficient fouling control was achieved by intermittent bubbling materials such as suspended particles, colloids and soluble
[288,289]. Pulsing air at a frequency of 1 s on/1 s off allowed an organics. In MBR-based trials, the addition of alum led to
improvement in operating flux ranging from 20 to 100% and was a significant decrease of the SMPc concentration, along with
found more efficient than lower frequencies (510 s on/510 s an improvement in membrane hydraulic performances [297].
off) more conventionally applied in the industry [288]. However, Because of back transport and shear induced fouling control
such system may require the operation of a robust activators and mechanisms, large microbial flocs are expected to have a lower
valves at these high frequencies and may not be economically impact on membrane fouling. The permeability enhancement
practical. observed for hybrid coagulant/MBR systems are therefore due to
the largest flocs formed. A recent MBR-based example reported
4.2.2.2. Other operating conditions. As mentioned before that small biological colloids (from 0.1 to 2 m) coagulated and
(Section 3.3.2), SRT remains probably the main operating formed larger aggregate when alum was added to MBR acti-
parameter defining the characteristics of the biomass suspension vated sludge [298]. Although more expensive, ferric chloride
and its fouling propensity. With the numerous reports defining was found to have higher efficiency than that of alum. Zeolite has
the relation between SRT and concentrations of both eEPS and also been used in MBRs and allowed the creation of rigid flocs
SMP, it appears that the overall performance of the MBR is that have lower specific fouling resistance. Further details about
closely related to the choice of SRT value. Further optimiza- the mechanisms of performance enhancement due to zeolite and
tions of operating conditions through reactor design have been alum can be obtained from [298]. The addition of ferric iron has
studied and include the addition of a spiral flocculator [290], also been tested on an MBR for enhancing the production of iron-
vibrating membranes [291], helical baffles [292], suction mode oxidizing bacteria, responsible for the degradation of gaseous
[97] and high performance compact reactor [293], novel types H2 S. In this study, specific ferric precipitate like ferric phos-
of air lift [104], porous and flexible suspended membrane car- phate and K-jarosite (K-Fe3 (SO4 )2 (OH)6 ) have been observed
riers [294] and the sequencing batch MBR [295] for example. to foul the membrane [299]. Pre-treatment of the effluent is also
Finally, the membrane module design remains another impor- possible and studies based on the pre-coagulation/sedimentation
tant parameter in the optimization of the MBR operation, and of effluent before its introduction in the bioreactor revealed the
fouling limitation offered by this technique. Obviously, pre- ing recoveries were observed (88% of those obtained with a
treatment of the feed is a crucial step in the MBR process. conventional MBR).
Fundamental of sieving, current state-of-the-art mechanical pre- A novel membrane performance enhancer (MPE 50) has been
treatment and results from the comparison between different recently developed by Nalco and applied to MBRs. When 1 g/l
types of sieves are given in [300]. In a recent example, the addi- of cationic polymer-based compound was added directly to the
tion of iron based coagulant controlled both irreversible fouling bioreactor, SMPc was found to decrease from 41 to 21 mg/l
and suspension viscosity [145]. Ferric hydroxide flocs have also [306]. The interaction between the polymer and the soluble
been used in the MBR process as a membrane pre-coating agent. organics in general, and SMPc in particular, was named as the
Not only the specific flux of this set up was higher, but the efflu- main mechanism responsible for the performance enhancement
ent quality was also improved compared to the non-coated MBR when Nalcos polymer was used. In another example, an MBR
system [280]. In this study, additional ferric chloride was added operated with MLSS as high as 45 g/l featured a lower fouling
to successfully remove the non-biodegradable organics which propensity when 2.2 g/l of polymer was mixed to the bioreactor.
accumulated in the bioreactor. This operation also led to a rapid Experiments conducted with different system configurations
increase in membrane specific flux. of submerged hollow fiber membranes allowed direct compar-
ison of hydraulic performances for pre-flocculation and PAC
4.2.3.2. Adsorbent agents. Addition of adsorbents into biologi- addition. Under the operating conditions used in this study, pre-
cal treatment systems decreases the level of pollutants, and more flocculation presented higher fouling mitigation than that of PAC
particularly organic compounds. When PAC is mixed with the addition [290]. However, when both strategies were used simul-
MBR biological suspension, biologically activated carbon forms taneously, membrane performances were maximum [290,307].
and is responsible for significant uptake of soluble organics. Dur-
ing long-term runs, PAC gradually incorporates to the biofloc 5. Conclusions
to form some biologically activated carbon [301]. Adsorption
of EPS on PAC has been studied during the comparison of After more than 10 years of intensive research, consensus
sidestream and submerged hybrid PAC-MBRs [302]. For this on the exact fouling phenomena in MBRs has not been reached
reason, lower fouling propensity is expected in MBR processes yet. Originally, it was suspected that aeration rate and MLSS
when biomass is mixed with adsorbents. Results conducted with concentration had the main impact on MBR fouling. Notwith-
only MBR supernatant also clearly revealed lower fouling when standing their significant effects, new areas of research have
PAC was added (up to 1 g/l) [303]. An optimum PAC concen- been since developed around the more detailed characterization
tration of 1.2 g/l was obtained for filtration of activated sludge of these parameters. Efforts now concentrate on optimizing air
[262]. In this study, floc size distribution and apparent viscosity distribution along the membrane modules and on more precise
of the biomass were the main factors responsible for the lower identification of the biological parameters, which have the most
cake resistance observed when PAC was added to the bioreactor. influence on the membrane performances. With the significant
However, no significant improvement of filtration was obtained changes in biomass characteristics from one plant to another, it
with the addition of 5 g/l of PAC and no sludge wastage [207]. It is not surprising to observe different biomass parameters affect-
was postulated that the originally introduced-PAC was quickly ing MBR fouling with various propensities. These disparities
saturated with organic pollutants. Only the regular addition of are also partly due to the different analytical methods and instru-
PAC into the bioreactor showed good fouling limitation, as the ments used in the reported studies. In other words, the quest for a
system was operated at lower SRT. Results reported by Fang et al. single fouling parameter in MBR seems in vain. A large number
[304] confirmed this hypothesis as virgin PAC was responsible of recent publications indicate the biomass supernatant (SMP)
for 22% reduction of the filtration resistance, while pre-sorbed and its carbohydrate fraction to be one of the main parameters
PAC only reduced the resistance by 14%. affecting MBR fouling. However, the more detailed characteri-
Finally, a detailed mathematical model considering sub- zation of the supernatant and the fouling layer currently carried
processes like biological reactions in the bulk liquid solution, out also reveals the significant role played by the protein fraction.
film transfer from bulk liquid phase to the biofilm, diffusion with The effect of pore size on membrane fouling is also crucial for
biological reaction inside biofilm, adsorption equilibrium at the MBR design, but the assessment of an optimized membrane pore
biofilmadsorbent interface, and diffusion within the PAC par- size is time-dependant. MF-based MBR systems seem to rely on
ticles has been proposed for predicting performances for hybrid initial fouling and the resulting creation of a dynamic membrane
PAC/MBR systems [305]. Numerous other studies reported the to produce high product quality, while UF-based MBRs feature
use of PAC for MBR fouling limitation, but generally failed to good rejection from the early stage of filtration. However, this
assess key issues such as extra operating cost and disposal of review revealed no clear advantage of using tight membranes
the elevated amount of sludge to be wasted. However, Ng et al. over more open pores (within a given flux range). Finally, the
recently assessed more clearly the long-term performances of filtration time (short-term versus long-term), the mode of opera-
such hybrid systems [301]. tion (constant flux versus constant TMP), the initial stage of the
In order to obtain higher biological aggregates in the biore- membrane (new versus cleaned), the operating conditions and
actor, aerobic granular sludge has also been used in MBR sys- the cleaning protocol are also crucial elements when the foul-
tems [144]. With an average size around 1 mm, granular sludge ing experiments are designed and should be carefully selected,
increased the membrane permeability by 50%, but lower clean- 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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Colloids: Very small, finely divided solids (particles that do not dissolve) that Hydraulic retention time (HRT): The HRT is equivalent to the theoretical deten-
remain dispersed in the aqueous phase due to their small size (from 1 nm to tion time for an ideal plug flow or completely mixed reactor and is calculated
1 m) and electrical charge. as the volume of bioreactor divided by the influent flowrate.
Conventional Activated Sludge Process (CASP): Process in which a clarifier Membrane bioreactor (MBR): Technology combining biological degradation
follows the aeration tank and is used for solids separation. process by activated sludge with a direct solidliquid separation by filtration.
Deposition: Settling of particles from a solution or suspension mixture on a Proteins: Chemical substances based on the polymerisation of amino acids. Dur-
pre-existing surface. ing biological degradation, proteins are hydrolysed to polypeptides, amino
Extracellular polymeric substances (EPS): Construction materials for microbial acids, and then ammonia and simple organic compounds.
aggregates such as biofilms, flocs and activated sludge liquors (see Section Solids residence time (SRT): The SRT (also called the mean cell residence time
3.2.5). or sludge age) is equivalent to the average time that microorganisms spend
Extracted extracellular polymeric substances (eEPS): Solution obtained after in the MBR and is calculated as the mass of organisms in the reactor divided
the physical and/or chemical extraction of the EPS from the biological walls by the mass of organisms generated/wasted from the reactor each day.
of the microorganisms. Soluble microbial products (SMP): SMP (also called soluble EPS or biomass
Fouling: Undesirable accumulation of (particulate, colloidal, molecular) mate- supernatant) are defined as soluble cellular components that are released
rials on the internal or external structure of the membrane. If the fouling during cell lysis, diffuse through the cell membrane, are lost during synthesis
involves living things such as microorganisms, the term biofouling may be or are excreted. In MBR systems, they can also be provided from the feed
used. substrate (see Section 3.2.6).