DES-12766; No of Pages 8

Desalination xxx (2015) xxx–xxx

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Desalination

journal homepage: www.elsevier.com/locate/desal

Effect of mechanical scouring by granular activated carbon (GAC) on membrane

fouling mitigation
Bing Wu a, Farhad Zamani a,b, Weikang Lim a, Dexiang Liao c, Yuanyuan Wang a,d, Yu Liu d,e,
Jia Wei Chew a,b,⁎, Anthony G. Fane a,d
a
Singapore Membrane Technology Centre, Nanyang Environment and Water Research Institute, Nanyang Technological University, 1 Cleantech Loop, CleanTech One #06-08, 637141, Singapore
b
School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, 637459, Singapore
c
College of Ocean Environment and Engineering, Shanghai Maritime University, Shanghai 201306, PR China
d
School of Civil and Environmental Engineering, Nanyang Technological University, 50 Nanyang Avenue, 639798, Singapore
e
Advanced Environmental Biotechnology Centre, Nanyang Environment and Water Research Institute, Nanyang Technological University, 1 Cleantech Loop, CleanTech One #06-08,
637141, Singapore

H I G H L I G H T S

• Effect of GAC size, membrane pore size, permeate flux and operation mode on fouling
• GAC improved the threshold flux values more for the larger membrane pore size.
• GAC increased the irreversible fouling resistance in the continuous filtration mode.
• Threshold flux and fouling layer resistance independent of GAC particle diameter
• New model with emphasis on mechanical scouring agrees with experiments.

a r t i c l e i n f o a b s t r a c t

Article history: The mitigation of membrane fouling due to the mechanical scouring behavior of granular activated carbon (GAC)
Received 13 August 2015 particles of diameters ranging from 0.9 to 4.6 mm was studied using a GAC tangential shear-membrane filtration
Received in revised form 1 October 2015 cell, wherein GAC was directed to scour the membrane surface by a magnetic stirrer placed 10 mm above the
Accepted 7 December 2015
membrane. Two membrane pore sizes (namely, 0.1 and 0.45 μm), two permeate fluxes (namely, an above-
Available online xxxx
and below-threshold flux) and two operation modes (namely, continuous and intermittent filtration) were in-
Keywords:
vestigated. Results indicated that: (1) GAC marginally improved threshold flux values, with the benefits more
Membrane fouling mitigation significant for the larger-pore membrane; (2) For continuous filtration, the presence of GAC reduced the cake
Granular activated carbon (GAC) layer resistance, but increased the irreversible resistance; (3) For intermittent filtration, GAC was surprisingly
Cake layer fouling less effective in reducing cake layer resistance compared to continuous filtration for the smaller-pore membrane,
Irreversible fouling but did not increase the irreversible fouling resistance; (4) Both threshold flux and fouling layer resistance were
Fouling resistance independent of GAC particle diameter, which contradicts the inertial lift model and thereby affirms the domi-
Mechanical scouring nance of the mechanical scouring behavior studied here; (5) A model developed, based on momentum transfer
between the GAC particle and foulant, provided a mechanistic understanding.
© 2015 Elsevier B.V. All rights reserved.

1. Introduction can be alleviated by effective fouling control strategies depending on

Membrane filtration is widely applied in water treatment and recla-
mation processes. However, membrane fouling, which results in an in-
crease of the energy required to maintain permeate production,
remains a key bottleneck. Although membrane fouling is inevitable, it
⁎ Corresponding author at: Singapore Membrane Technology Centre, Nanyang
Environment and Water Research Institute, Nanyang Technological University, 1
Cleantech Loop, CleanTech One #06-08, 637141, Singapore.
E-mail address: JCHEW@ntu.edu.sg (J.W. Chew).
the type of fouling that is operative (e.g., cake versus pore plugging; re-
versible fouling or irreversible fouling; particle-dominant fouling or sol-
uble substance-dominant fouling; organic fouling or inorganic fouling,
etc.). If cake layer fouling is predominant, periodic physical cleaning
methods (including backwash, mechanical, hydraulic and pneumatic
approaches, vibration, sonication, etc.) are generally suggested to main-
tain the membrane performance [1]. Among these membrane cleaning
approaches, the addition of scouring particles to either interfere with
the cake layer formation or to remove the formed cake layers has
been proven to enhance membrane filtration due to mechanical

http://dx.doi.org/10.1016/j.desal.2015.12.003
0011-9164/© 2015 Elsevier B.V. All rights reserved.

Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
2 B. Wu et al. / Desalination xxx (2015) xxx–xxx
abrasion forces and an increase of shear-induced diffusion along the
membranes [2,3].
Several types of scouring particles (such as plastic suspended car-
riers [2,4,5,6], powdered activated carbon (PAC) [7,8,9] and granular ac-
tivated carbon (GAC) [10,11,12,13,14]) have been studied and found to
enhance membrane permeability in microfiltration (MF), ultrafiltration
(UF) or membrane bioreactors (MBRs). Among these scouring agents,
PAC and GAC particles have been more popularly integrated with mem-
brane filtration due to their additional adsorption capability. Compared
to PAC, the larger-sized GAC is more easily retained in the reactor. Also,
by virtue of its larger size, GAC has a flow trajectory more independent
from the liquid flow field and hence stronger physical interactions with
the membrane surface.
In a few past studies, the scouring efficacy of GAC has been
harnessed by employing either gas–liquid-solid [15,16] or liquid–solid
[17] fluidization, wherein the membrane mitigation effects conferred
by GAC were contributed by both the mechanical scouring mechanism
and particle back-transport mechanism. It should be noted that the me-
chanical scouring mechanism is somewhat different from the particle
back-transport mechanism [18], although both alleviate membrane
fouling. While the former supposes the GAC particle to be in intimate
contact with the membrane, the latter on the contrary predicts that
the millimeter-size GAC particles are likely not to be in contact with
the membrane due to inertial lift. However, the two contributions are
not easily distinguished during fluidization. In addition, although the
extent of fouling mitigation has been reported to be positively correlat-
ed with both GAC particle diameter and concentration [19], whether the
beneficial effect is rooted in mechanical scouring or particle back-
transport is unclear. Therefore, the goal of the current effort is twofold:
(1) to experimentally determine the impact of mechanical scouring,
with minimal influence of particle back-transport, on membrane fouling
mitigation, and (2) to understand the relationship between GAC particle
diameter and mechanical scouring efficacy.
To focus only on the mechanical scouring effects, since the inertial
lift phenomenon is rather well studied [18], a tangential shear filtration
cell was designed and used in this study to ensure that the GAC particles
were consistently in intimate contact with the membrane. Specifically,
the GAC was induced to tangentially scour the membrane surface by a
magnetic stirrer placed 10 mm above the membrane. Under such condi-
tions, the GAC scouring mechanism, rather than the inertial lift mecha-
nism, predominates in mitigating fouling. A feed mixture composed of
bovine serum albumin, sodium alginate, humic acid, and bentonite
was used to simulate the complex foulants in the mixed liquor of a bio-
reactor. The extent of fouling (in terms of cake layer resistance and foul-
ing rate) was compared in the absence and presence of GAC particles of
various sizes. Furthermore, a mechanistic model was developed to pro-
vide a physical understanding of the relationship between the effective-
ness of GAC scouring and GAC particle diameter. This study provides
insights and guidance on the effects of GAC particle diameter,
membrane pore diameter, permeate flux and operation mode
(i.e., continuous versus intermittent filtration) in the employment of
GAC scour to mitigate membrane fouling.
2. Materials and methods
2.1. Model foulant solution
The model foulant suspension was formulated to simulate the com-
plex effluent of an anaerobic bioreactor, which typically contains pro-
teins, polysaccharides, humic substances, and particles. Accordingly,
bovine serum albumin (BSA, 100 mg/L, Sinopharm Chemical Reagent
Co. Ltd., China), sodium alginate (SA, 100 mg/L, Hanawa Chemical,
Japan), humic acid (HA, 100 mg/L, Aldrich-Sigma, USA), and bentonite
(100 mg/L, Aldrich-Sigma, USA) were used to represent protein,
polysaccharides, humic substances, and particles in wastewater,
Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
respectively. The characteristics of the model compounds are described
in the supplementary data (Table S1 and Figure S1).
2.2. Membrane filtration setup
A bench-scale stirred filtration setup was used to investigate the
scouring behavior of GAC (Fig. 1). Specifically, a virgin hydrophilic
polyvinylidene fluoride (PVDF) membrane (0.00125 m2 of surface
area) was aligned horizontally at the bottom of a 100 mL filtration cell
and a magnetic stirrer bar (effective length of 26 mm) was located
10 mm above the membrane surface to induce the tangential move-
ment of the GAC particles. Two types of hydrophilic PVDF membranes
differing only in nominal pore sizes (namely, 0.1 μm and 0.45 μm)
were purchased from Merck Millipore (USA). The rotation speed of
the stirrer bar was fixed at ~ 150 rpm (equivalent to an average shear
rate of ~10 s−1), which ensured that GAC particles (at a concentration
of 0.4 g in 100 ml liquid) moved along the membrane surface, thereby
inducing a tangential particle-induced shear effect. Although some
GAC particles can be expected to move axially in the cell due to inter-
particle collisions, the dominant motion was tangentially due to the tan-
gential flowfield generated by the stirrer. It was assumed reasonably
that the particle scour was significantly greater than liquid shear effects
in this set-up. The feed solution was pumped to the filtration cell in
order to maintain a constant water level in the cell, while the permeate
flow rate was regulated by another pump (Cole-Parmer, USA). The per-
meate was collected in a beaker where its weight was measured by an
electronic balance (Mettler-Toledo, Switzerland) to compute the per-
meate production rate. The trans-membrane pressure (TMP), which is
the difference between the feed and permeate pressures, was measured
by pressure transducers (Cole-Parmer, USA). Data from the electronic
balance and transducers were logged on a personal computer equipped
with Labview (National Instruments, USA).
The GAC was purchased from Sigma-Aldrich (USA). Specifically, the
GAC is Norit GAC, which originated from untreated peat bog, and has a
surface area of 600–800 m2/g. Two size ranges of GAC were purchased,
namely 0.9–2 mm (particle density of approximately 280 kg/m3) and
2.4–4.6 mm (particle density of approximately 320 kg/m3). Five subsets
of GAC were obtained by sieving: GS1 (0.9–2 mm), GS2 (2–2.4 mm),
GS3 (2.4–3.4 mm), GS4 (3.4–4 mm), and GS5 (4–4.6 mm). It is recog-
nized that, although the particle concentration was kept constant at
0.4 g/100 ml, the different particle diameters resulted in different num-
ber of particles and different specific surface area. However, in practical
applications, the GAC concentration and particle diameters are two pa-
rameters which could be easily quantified, rather than particle number
and specific area, hence we have chosen the former two for this study.
Fig. 2 depicts the morphologies and size differential of the various
sieve fractions. Before each experiment, the fresh GAC particles were
washed with distilled water to displace the trapped air within the GAC
particles with water and to remove the fine carbon powder loosely at-
tached on GAC particles.
2.3. Threshold flux determination
The concept of ‘critical flux’, which defines the minimum flux at
which deposition starts, is not strictly applicable for multiple-
component feeds; because each component has its own critical flux,
the multiple-component feed has instead a range of critical fluxes. In
such cases, it is more meaningful to determine a ‘threshold flux’,
which is the flux value that demarcates a region of low fouling rate
from a high fouling rate [20,21,22]. The threshold flux of the model mix-
ture was determined using the following protocol: (1) the flux was in-
crementally increased at 15 min intervals, (2) the slope of the TMP
profile (d(TMP)/dt) was computed at each flux step, and (3) the thresh-
old flux, at which the regression lines of the low fouling region and the
high fouling region intersect, was determined. In order to minimize var-
iations due to GAC adsorption, the GAC particles were saturated with
 B. Wu et al. / Desalination xxx (2015) xxx–xxx
Fig. 1. A schematic diagram of GAC tangential shear-membrane filtration setup.
the model foulant solution before the threshold flux tests. According to
the adsorption kinetics plot generated in the Results and Discussion sec-
tion (Fig. 5), the GAC particles were fully saturated beyond 1 h.
2.4. Membrane fouling resistance and fouling rate
The resistance of the fouling layer on the membrane, R, was used to
evaluate the impact of the five diameters of GAC on the filtration pro-
cess. R is calculated by the equation: R = TMP/(μpJ), where μp is the per-
meate viscosity and J is permeate flux. Two permeate fluxes (namely, 14
and 32 LMH) were employed in this study. Three steps were performed
to determine the TMP: (i) the TMP of the clean membrane (TMPm)
was measured by using distilled water for 10 min, (ii) TMPm + reversible +
irreversible, which was measured using the model foulants, embodies the
TMP that corresponds to the membrane and both the reversible and ir-
reversible fouling, and (iii) TMPm + irreversible, which was measured by
using distilled water after the fouled membrane had been rinsed with
distilled water. For each condition, triplicate experiments were per-
formed using fresh GAC (i.e., after the washing protocol described in
the ‘membrane filtration setup’ section). The averaged results and stan-
dard deviations (shown as error bars) are presented in the figures. The
filtration experiments with and without the addition of GAC were con-
ducted, where the latter served as a control experiment.
2.5. Adsorption kinetics of GAC particles
The adsorption kinetics of the GAC particles were measured as fol-
lows: (1) prepare the suspensions, each of which consisted of 100 ml
of model foulant solution and 0.4 g GAC particles, and (2) at regular in-
tervals, sample 10 mL of solution, filter with a 0.45 μm filter (Pall Corpo-
ration, US), and measure the total organic carbon (TOC) by a TOC
analyzer (Shimadzu, Japan).
2.6. Membrane morphology observation
After 2 h of filtration at a flux of 32 L/m2 h (LMH), the membrane was
carefully removed from the filtration cell and pre-treated using a
Heraeus vacuum oven (Thermo Scientific, USA) at 40 °C for 15 h to re-
move the moisture content. After the membrane was sputter-coated
with gold, a field emission scanning electronic microscope (FESEM,
Fig. 2. Morphologies of GAC used in this study.
Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
3
JEOL, Japan) was used to characterize the membrane surface
morphology.
2.7. Model foulant solution and permeate analysis
Three characterization analyses were carried out on the model
foulant solution, membrane foulants and permeate: (i) the TOC values
of the model foulant solution and permeate were analyzed by a TOC an-
alyzer (Shimadzu, Japan), (ii) the particle sizes of the model foulant so-
lution and permeate were measured by a zetasizer (Malvern, UK), and
(iii) the turbidity of model foulant solution was determined by a turbid-
ity meter (Hach, USA).
3. Results and discussion
3.1. Effect on fouling resistance
The dTMP/dt at each filtration flux was determined in order to iden-
tify the threshold flux, as shown in Fig. 3. On one hand, for the mem-
brane with a nominal pore size of 0.1 μm, the threshold flux values
were very similar in the absence and presence of GAC at 18 and 19
LMH, respectively. On the other hand, for the membrane with a nominal
pore size of 0.45 μm, the threshold flux value was improved in the pres-
ence of GAC, giving threshold flux values in the absence and presence of
GAC of 27 and 31 LMH, respectively. Surprisingly, at each membrane
pore size, the five particle diameters of GAC resulted in approximately
the same threshold flux values, which imply that the extent of scouring
was independent of the particle diameter of GAC. This affirms that me-
chanical scouring, instead of inertial lift, which would have particle di-
ameter dependence, is the dominant mechanism.
To further explore the impact of GAC on scouring, the membrane fil-
trations were performed at two fluxes of 32 and 14 LMH, which were re-
spectively above and below the measured threshold flux of the model
foulant suspension investigated (Fig. 3). To obtain the same order of
magnitude for the total resistance of the fouling layer, the filtration pe-
riod was 2 h and 16 h at the flux of 32 LMH and 14 LMH, respectively.
Fig. 4A presents the resistances of the cake layer (i.e., reversible fouling)
and irreversible fouling layer for the two membrane pore sizes at the
above-threshold flux of 32 LMH, while Fig. 4B shows that for the
below-threshold flux of 14 LMH. The cake resistance was dominant at
95.1 ± 5.8% and 85.9 ± 15.6% of the total resistance for the fluxes of
32 and 14 LMH, respectively. GAC reduced the cake resistance by
35.4 ± 13.0% and 44.2 ± 25.8% for the fluxes of 32 and 14 LMH, respec-
tively. In view of the large standard deviations, presumably due to the
well-acknowledged variations among membranes even from the same
batch, a two-sample T-test was further carried out. In this case, the
resulting p-value was b0.1, which indicates that the difference between
the two cake resistances was statistically significant at a confidence
4 B. Wu et al. / Desalination xxx (2015) xxx–xxx

Fig. 3. Effect of GAC particle diameter on threshold flux. Fig. 4. Effect of GAC particle size on fouling resistance at (A) an above-threshold flux of 32
LMH (filtration duration of 2 h), and (B) a below-threshold flux of 14 LMH (filtration du-
level of 90%. On the other hand, except for the case of 0.1 μm membrane ration of 16 h).
pore and 32 LMH flux whereby the impact of GAC on irreversible fouling
was negligible (Fig. 4A), GAC increased the irreversible cake resistance
more significantly for the 0.45 μm membrane pore and 14 LMH flux
by up to 27.0% (Fig. 4B). Similar to the lack of correlation between
GAC particle diameter and threshold flux exhibited in Fig. 3, the fouling
layer resistance was also independent of GAC particle diameter (Fig. 4).
The increase of irreversible fouling by GAC warrants a closer inspec-
tion. A plausible cause lies in adsorption capacity, especially in view of
the 8-fold longer filtration duration at the lower 14 LMH flux (Fig. 4B).
However, Fig. 5 shows that the adsorption capacity of GAC was saturat-
ed after 1 h of contact with the model foulant solution, thus indicating
that adsorption by GAC for filtration durations beyond 1 h was negligi-
ble and thereby would not have caused the difference in irreversible
fouling. Alternatively, the difference in irreversible fouling resistance
may be traced to the release of fine particles by GAC, which in turn act
as foulants. It should be noted that the GAC particles were washed off
of fines before each experiment, hence the fines observed were released
during the experiments. Fig. 6A shows that relative turbidity, which in-
creased by approximately 20–30 NTU due to the fines released after a
filtration duration of 2 h, was not related to GAC particle diameter. Fur-
thermore, Fig. 6B depicts the particle size distributions of the fine parti-
cles, whose diameters were in the range of 40–1800 nm. No correlation
existed between the mean particle sizes of the fine particles (Fig. 6B)
and GAC particles used (Fig. 2). The fine GAC particles released may
block the membrane pores, thereby increasing the irreversible fouling Fig. 5. Adsorption kinetics of model foulant solution by GAC particles.

Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
 B. Wu et al. / Desalination xxx (2015) xxx–xxx 5

Fig. 6. (A) Relative turbidity of the feed after 2 h at 32 LMH. Relative turbidity provides an indication of the amount of fine carbon particles released during filtration, and was determined by
the difference between the turbidity of the model foulant solution in the presence and absence of GAC. (B) Particle size distribution of the fines released.

particularly for the membrane with the larger 0.45 μm pore (Fig. 4A and
B). Moreover, the released fine particles surprisingly had a greater im-
pact at the lower 14 LMH flux, presumably because the relatively slower
cake layer formation allowed more opportunities for fine particles to in-
teract directly with and be irreversibly attached to the membrane. As is
well-acknowledged, the cake layer serves as a secondary membrane to
protect the membrane from internal fouling. The lack of a correlation
between turbidity and GAC particle diameter observed in Fig. 6B agrees
with the similar lack of impact of GAC particle diameter on increasing
the irreversible fouling.
To understand the different threshold flux and fouling layer resis-
tance values, respectively, due to the different membrane pore sizes,
SEM images of the fouled membranes were taken. Although GAC parti-
cles improved the threshold flux only slightly (Fig. 3), they were able to
reduce the cake layer resistance by at least 35% (Fig. 4), which indicates
that the nature of the cake is important to the effectiveness of GAC
scouring. The differences observed via SEM images of the cake structure
hence were expected to shed some light on the underlying fouling mit-
igation. Fig. 7 shows the fouled membrane (at the end of 2 h of contin-
uous filtration at 32 LMH) in the absence and presence of GAC for the
two membrane pore sizes of 0.1 and 0.45 μm investigated. In the ab-
sence of GAC (Fig. 7A and C), the cake surface morphology for both
membrane pore sizes were relatively similar. However, in the presence
of GAC (Fig. 7B and D), a more porous cake morphology resulted only for
the 0.45 μm membrane. The difference in the porosity of the cake layer
is possibly because the employed flux of 32 LMH was much higher than
the threshold flux for the 0.1 μm membrane (18–19 LMH; Fig. 3A), but
only slightly higher than that for the 0.45 μm membrane (27–31 LMH;
Fig. 3B). Therefore, the cake layer tended to be denser on the 0.1 μm
membrane, which explains (i) the larger differential between the
threshold flux values in the absence and presence of GAC for the
0.45 μm membrane, because the porous cake layer was more easily re-
moved by GAC scouring, and (ii) the more extensive increase of the
irreversible fouling layer resistance for the 0.45 μm membrane (Fig.
4A), because the more porous cake layer in the presence of GAC allowed
for easier irreversible deposition of the GAC fines on the membrane. It
should be noted that this trend may be unique to this model foulant so-
lution, since the density of the cake layer and hence effectiveness of GAC
scouring may be different for a different foulant mixture.
The impact of GAC particle diameter on intermittent filtration was
also investigated, since relaxation (i.e., temporary cessation of flux) is
considered an effective approach to alleviate cake layer fouling. Both
in the absence and presence of GAC particles, the intermittent filtration
was operated such that 32 LMH was implemented for 9 min, followed
by 1 min of relaxation (i.e., without filtration) repeatedly until the
total filtration duration at 32 LMH was 2 h. Analogous to Fig. 4, the
membrane fouling resistances for the intermittent filtration mode of op-
eration are presented in Fig. 8. Similar to Fig. 4 for continuous filtration,
the cake resistance in Fig. 8 for intermittent filtration was also the dom-
inant resistance at 92.9 ± 5.2% of the total resistance. Consistent with
previous observations, the impact of GAC particle diameter was insignif-
icant. Dissimilar to Fig. 4B, Fig. 8 shows that for intermittent filtration,
(i) the reduction of cake layer resistance in the presence of GAC was
half that for continuous filtration for the 0.1 μm membrane, but GAC
was just as effective for the 0.45 μm membrane, and (ii) the irreversible
fouling resistance value for both the presence and absence of GAC were
similar, which implied that GAC did not increase irreversible fouling for
both membranes. Observation (i) suggests that GAC scouring was sur-
prisingly more effective in the continuous filtration mode compared to
the intermittent filtration mode, but only for the 0.1 μm membrane,
may be tied to the binding of the fine particles to the cake layer in the
absence of GAC scouring during relaxation. This is consistent with the
hypothesis earlier that the fines increased irreversible fouling at the
lower flux due to slower cake formation; along the same vein, internal
fouling by fines affected the smaller 0.1 μm pores more significantly. Ob-
servation (ii) indicates that the short relaxation duration was sufficient

Fig. 7. SEM images of cake layers on the membranes after 2 h of continuous flux at 32 LMH.

Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
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6 B. Wu et al. / Desalination xxx (2015) xxx–xxx
Fig. 8. Effect of GAC particle size on fouling resistance under the intermittent filtration
mode (i.e., 9 min of 32 LMH, followed by 1 min of relaxation).
to effectively eliminate irreversible fouling, presumably by causing the
fine particles to detach from the membranes. It should be noted that ir-
reversible resistance in this case was similar to that in the absence of
GAC for both membranes, despite the 0.45 μm membrane having
much more extensive irreversible fouling relative to the 0.1 μm mem-
brane for the continuous filtration mode (Fig. 4B).
After continuous filtration was implemented at 32 LMH for 2 h, the
permeate was analyzed for particle size distribution (PSD) and total or-
ganic carbon (TOC). Fig. 9 presents the PSD profiles and TOC of the per-
meate obtained using the 0.1 μm membrane for the five GAC particle
diameters. As seen in Fig. 9A, the presence of GAC particles led to left-
ward shifts of the PSDs in the permeate, which was due to the fine
(nano-scale) carbon particles released from GAC that passed through
the membrane. The mean size of the fine particles in the permeate
had no apparent correlation with the particle diameter of the GAC
used. Fig. 9B shows that the TOC levels both in the presence and absence
of GAC particles were similar in the permeate at the end of the filtration
tests, which indicates that GAC scouring did not affect the integrity of
the membrane. Note that, because GAC adsorption was saturated at ap-
proximately 1 h (Fig. 5), the capability of GAC to further adsorb organic
carbon foulants was negligible beyond 1 h.
Fig. 9. Effect of GAC particle size on (A) the permeate particle size distribution (PSD) and (B) the permeate TOC. The results here were obtained at the end of 2 h of continuous filtration at
32 LMH with the 0.1 μm membrane.
Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
3.2. A simple model for a mechanistic understanding of the scouring
behavior
It should be noted that only mechanical scouring effects are
accounted for in this model. Adsorption effects by the GAC are not fac-
tored in, since fully saturated GAC particles were used in the experi-
ments. The filtration flux through the membrane exerts a drag force
on each foulant particle near the membrane surface. The drag force,
which can also be referred to as the deposition force (Fd) in this case,
causes foulants to deposit on the membrane. Fd is exerted on any parti-
cle in the concentration polarization layer and behaves like a force field
that attracts any particle towards the membrane surface, as illustrated
in Fig. 10. Assuming reasonably that the density of the foulants is similar
to that of water, the gravity and buoyancy forces counter-balance each
other, hence the only force acting on the foulants would be the Stokes
drag force. Accordingly, Fd can be calculated using the Stokes law for
laminar flow and spherical particles:
Fd ¼ 3 π μ d u f ð1Þ
where μ is the viscosity of the fluid, d is the diameter of the particle and
uf is the filtration flux velocity normal to the surface.
For a particle deposited at the membrane surface, the shear force due
to the crossflow liquid exerts a tangential drag force (Ft) on the particles,
as depicted in Fig. 11A. If Ft exceeds the attractive force between the par-
ticle and the membrane surface, the particle would detach from and
move along the membrane surface [23,24]. In the case whereby the par-
ticle does not enter the membrane pore, and the attractive force be-
tween the particle and the surface is weaker, as is the case in cake
layer fouling, the particle moves along the surface with the velocity of
the shear flow exerted at its center of mass (uc), as shown in Fig. 11B
[25]. Based on the reasonable assumptions that (i) the shear flow is lin-
ear close to the membrane surface, and (ii) the velocity is approximately
zero at the membrane surface (i.e., no-slip condition), uc is proportional
to the particle diameter (d), as illustrated in Fig. 11B. This in turn implies
that the larger-sized particles have larger velocities along the mem-
brane surface in the presence of laminar shear. In the context of this
study, because the GAC particles are on the millimeter-scale while the
foulant particles are much smaller on the micrometer- or nanometer-
scale, uc,GAC is orders-of-magnitude greater than uc,foulant.
In order to curb fouling, implementation of force fields opposing the
attractive force field due to the permeate flux (Fig. 10) is required. Spe-
cifically, the opposing force field needs to induce on the foulant particle
a velocity of at least the escape velocity (uescape), which is a hypothetical
velocity above which the particle is able to escape from the attractive
force field (Fig. 10). It should be noted that the mass of the GAC particle
 B. Wu et al. / Desalination xxx (2015) xxx–xxx
Fig. 10. The force field near a membrane surface with permeation.
is greater than that of the foulant (i.e., mGAC N mfoulant) and
uc,GAC N uc,foulant, hence the momentum of the GAC particle is significant-
ly greater than that of the foulant (PGAC N N Pfoulant). Because the stirrer in
this filtration setup ensured that the GAC particles at the membrane sur-
face moved at uc,GAC tangentially along the membrane surface, when a
GAC particle collides with a smaller foulant particle in its path, the
foulant particle acquires a velocity of uc,GAC as it is moved along by the
faster-moving GAC particle. For the foulant particles, uc,GAC can be larger
than uescape,foulant such that the foulant particles are ejected from the sur-
face. Although uc is tangential to the surface, the trajectory of particles
may be changed through collisions with other particles or the mem-
brane surface roughness elements. Thus, the foulant particles are re-
pelled from the membrane surface.
Physically, the scouring mechanism of GAC particles is based on the
momentum transferred from the GAC particles to the foulant particles
(Ptr). Ptr is linearly proportional to the product of the area scoured by
each GAC particle (A), the total number of GAC particles (NGAC) and
the velocity of the GAC particle (uc,GAC):
P tr ∝A∙NGAC ∙uc;GAC :
The scouring of foulant particles from the membrane surface by GAC
particles is shown schematically in Fig. 12, and accordingly A can be cal-
culated as:
A ¼ w∙t∙uc;GAC
where w is the effective width of the GAC particle (which hence is pro-
portional to dGAC) and t represents contact duration. Because uc,GAC is
proportional to dGAC (Fig. 11B), combining Equations (2) and (3) gives:
3
P tr ∝dGAC ∙NGAC ∙t:
Fig. 11. (A) The tangential force acting on a deposited particle (foulant or GAC) due to the induced shear, and (B) The positive correlation between the velocity of a particle at its center of
mass (uc) and the diameter of the particle (d).
Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
7
Fig. 12. A schematic depicting the area scoured by a GAC particle.
Since dGAC 3 is a measure of the particle volume, the term dGAC ∙NGAC
3
is proportional to the total volume of all the GAC particles at the mem-
brane surface. Therefore, Ptr is proportional to the total mass of GAC par-
ticles at the membrane surface, rather than the particle diameter (dGAC)
or the number of particles (NGAC) per se. Due to the particle back-
transport phenomenon [18], some of the GAC particles would rise and
establish a polarization layer near the membrane surface. It can be
shown that in such a system, the polarization profile of GAC particles
is also independent of dGAC and is only a function of the total mass of
3
GAC particles (i.e., dGAC ∙NGAC ) at the membrane surface. This behavior
is described in Appendix 1. The analysis is in agreement with the exper-
imental results, which showed that, when GAC mass concentration was
kept constant, the impact of the GAC particles on membrane fouling was
ð2Þ
independent of GAC particle diameter (dGAC).
4. Conclusions
This study demonstrates the tangential scouring capacity of five di-
ð3Þ
ameters of GAC particles (ranging from 0.9–4.6 mm) on a membrane fil-
tration process. The GAC particles were induced to tangentially shear
the membrane surface by a magnetic stirrer located 10 mm above the
membrane surface. Two PVDF membranes of different nominal pore
sizes (namely, 0.1 and 0.45 μm) were investigated. The threshold flux
values were first obtained, then filtration tests at above- and below-
ð4Þ threshold fluxes were carried out.
8 B. Wu et al. / Desalination xxx (2015) xxx–xxx
Through studying the effect of GAC particle diameter, permeate flux,
membrane pore size and operation mode (i.e., continuous versus inter-
mittent filtration), this effort provides a more in-depth understanding
on the impact of GAC on mitigating membrane fouling when mechani-
cal scouring is dominant. The lack of impact of GAC particle diameter in-
dicates that mechanical scouring, rather than the size-dependent
particle back-transport, was the dominant mechanism. A few highlights
are worth noting:
(1) GAC improved threshold flux values slightly, with the improve-
ment more significant for the larger membrane pore size;
(2) For continuous filtration, the presence of GAC (a) reduced the
cake layer resistance by at least 35% relative to that without
GAC, but (b) increased the irreversible resistance by up to 27%,
with the 0.45 μm membrane more significantly affected in part
due to a more porous cake morphology;
(3) Relative to continuous filtration, intermittent filtration gave dis-
similar results in that: (a) GAC was less effective in reducing
cake layer resistance for the 0.1 μm membrane, but not for the
0.45 μm membrane, and (b) GAC did not increase the irreversible
fouling resistance;
(4) Both threshold flux and fouling layer resistance were independent
of GAC particle diameter. The seeming contradiction between this
study and the previous experimental results [19] stems from me-
chanical scouring being the dominant mechanism in the former,
while mechanical scour, particle back-transport and other hydro-
dynamics effects were concurrently present in the latter.
(5) A model was developed to provide a mechanistic understanding
on the scouring behavior, based on the momentum transfer be-
tween the larger GAC particle and the foulant on the membrane
surface. Both the model and experiments agreed on the negligible
impact of GAC particle diameter on membrane fouling at the same
GAC concentration.
Acknowledgments
This study was supported by research grant (1102-IRIS-02-01) pro-
vided by the Singapore National Research Foundation under its Environ-
mental & Water Technologies Strategic Research Program and
administered by the Environment & Water Industry Program Office
(EWI) of the PUB. The Economic Development Board of Singapore
(EDB) is also acknowledged for funding the Singapore Membrane Tech-
nology Centre (SMTC), Nanyang Technological University (NTU). In ad-
dition, we acknowledge funding from NTU iFood Research grant
(M4081465.120) and Singapore Ministry of Education Academic Re-
search Fund Tier 2 (MOE2014-T2-2-074, ARC16/15). We also thank
Jillinda Toh and Steven Limbara from Republic Polytechnic for their ef-
forts in the lab.
Appendix A. Supplementary data
Supplementary data to this article can be found online at http://dx.
doi.org/10.1016/j.desal.2015.12.003.
Please cite this article as: B. Wu, et al., Effect of mechanical scouring by granular activated carbon (GAC) on membrane fouling mitigation, Desa-
lination (2015), http://dx.doi.org/10.1016/j.desal.2015.12.003
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