Water Research 212 (2022) 118098

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Water Research
journal homepage: www.elsevier.com/locate/watres

Insights on fouling development and characteristics during different fouling

stages between a novel vibrating MBR and an air-sparging MBR for
domestic wastewater treatment
Chuansheng Wang a, Tze Chiang Albert Ng a, b, 1, *, Meiyue Ding a, b, How Yong Ng a, b, 1, *
a
Centre for Water Research, Department of Civil and Environmental Engineering, National University of Singapore, 1 Engineering Drive 3, 117580 Singapore
b
National University of Singapore Environmental Research Institute, 5A Engineering Drive 1, 117411 Singapore

A R T I C L E I N F O A B S T R A C T

Keywords: Membrane fouling remains a major hindrance to a prevalent application of membrane bioreactor (MBR) for
Vibrating membrane bioreactor wastewater treatment. Vibrating membrane technology has recently attracted increasing attention in energy-
Fouling control efficient fouling control in MBR compared to air sparging. However, little is known about its fundamental
Fouling development
fouling control mechanism and whether the vibrating MBR (VMBR) is a highly effective strategy to control
Dissolved organic matters
Domestic wastewater
fouling constitutions and fouling sources compared to the conventional air-sparging MBR (ASMBR). This study
operated two parallel MBRs with vibrating or air-sparging membrane modules for long-term (215 d) real do­
mestic wastewater treatment. Effects of air sparging and vibration rates on fouling control, fouling development
and fouling sources across three fouling stages were comprehensively evaluated. Results showed that the VMBR
achieved 70% lower fouling rates compared to the ASMBR due to a remarkable retardation in each fouling stage
by membrane vibration. The VMBR significantly reduced over 62.7% of colloidCL and SMPCL within the cake
layer (CL) to simultaneously alleviate the reversible and irreversible fouling compared to the ASMBR. The
comparatively lower dissolved organic matter (DOM) and biopolymer contents in the cake layer of the VMBR
resulted in a slower TMP rise. The main DOMs in the foulants of both MBRs were found in the following order:
aromatic protein > soluble microbial by-products > other organics. EPSML from mixed liquor (ML) contributed
more DOMs to form membrane foulant than the SMPML in both MBRs. Aromatic proteins and soluble microbial
products in the EPSML were markedly reduced in the VMBR but increased in the ASMBR in high-shear phase,
demonstrating higher effectiveness in fouling control by membrane vibration. This study provided insights into
understanding fouling control, fouling development characteristics and fouling mechanisms between the VMBR
and ASMBR, which might guide the researchers and engineers to apply novel vibrating MBRs to better control
membrane fouling for holistic wastewater treatment in full scale.

EPSCL EPS in the cake layer

Abbreviations EPSML EPS in the mixed liquor
ASMBR Air sparging membrane bioreactor HRT Hydraulic retention time
ColloidCL Colloids in the cake layer LC–OCD Liquid chromatography organic carbon detector
ColloidML Colloids in the mixed liquor LMW Low molecular weight compound
DO Dissolved oxygen MBR Membrane bioreactor
DOC Dissolved organic carbon PS Polysaccharide
DOM Dissolved organic matter PN Protein
DWW Domestic wastewater SMP Soluble microbial product
EEM Excitation emission matrix SMPCL SMP in the cake layer
EPS Extracellular polymeric substances SMPML SMP in the mixed liquor

* Corresponding author.
E-mail addresses: albert.n@nus.edu.sg (T.C.A. Ng), howyongng@nus.edu.sg (H.Y. Ng).
1
Please list both Tze Chiang Albert Ng and How Yong Ng as corresponding authors

https://doi.org/10.1016/j.watres.2022.118098
Received 19 October 2021; Received in revised form 11 January 2022; Accepted 17 January 2022
Available online 18 January 2022
0043-1354/© 2022 Elsevier Ltd. All rights reserved.
C. Wang et al.
SRT Solid retention time
SS Suspended solids
SWW Synthetic wastewater
TMP Transmembrane pressure
VMBR Vibrating membrane bioreactor
VSS Volatile suspended solids
1. Introduction
Membrane bioreactor (MBR) has become an attractive technology
for domestic wastewater (DWW) treatment due to its advantages of
complete biomass retention and high-quality effluent compared to
conventional activated sludge process (Judd, 2008; Ng et al., 2020).
However, membrane fouling remains a major issue for long-term and
economic viability of MBRs. Mitigating and understanding membrane
fouling has invariably been of great interest to researchers and engineers
for improving MBR technology (Bagheri and Mirbagheri, 2018; Hamedi
et al., 2019). Without introducing chemical or biological additives,
in-situ physical shear-enhanced method such as air sparging coupled
with relaxation and backwash is typically used as the main method to
control fouling in pilot- and full-scale MBRs (Kimura et al., 2005; Miura
et al., 2007; Xiao et al., 2019). However, in air-sparging MBRs
(ASMBRs), high aeration intensity not only requires over half of the
energy demand in an MBR process, but also disrupts the biomass flocs to
release smaller-sized particles resulting in an unfortunate trade-offs for
fouling control (Belli et al., 2021; Fan and Zhou, 2007; Meng et al.,
2008). Recently, membrane vibration or reciprocation has been devel­
oped as a novel shear-enhanced method applied in-situ fouling control
(Bilad et al., 2012; Ho et al., 2014; Kaya et al., 2020; Kola et al., 2014;
Wang et al., 2021). In a vibrating MBR (VMBR), shear stress enhanced
by membrane vibration could detach the foulants from the membrane
surface to control fouling (Bilad et al., 2012; Wang et al., 2014). Such a
configuration has been reported to save up to 78.5% energy demands of
air sparging in MBR technology treating DWW (Wang et al., 2021). Yet,
very few studies reported the fundamental fouling control mechanisms
of the VMBR compared to the ASMBR, and little was known on whether
this novel technology would be a highly effective alternative to the
conventional energy-intensive ASMBR for controlling foulant formation
and its sources.
Hydrodynamic shear generated by air sparging in the ASMBR miti­
gated membrane fouling by minimizing the effects of concentration
polarization and floc deposition but was ineffective in removing the cake
(gel) layer and pore blockage (Le-Clech et al., 2006; Wang et al., 2014).
Whether membrane vibration in the VMBR can effectively alleviate the
cake layer formation and pore blockage is still under investigation. An
in-depth analysis of foulant formation along with fouling development
between novel VMBR and ASMBR is critical to explore the similarities
and differences in their fouling control mechanisms. Le-Clech et al.
(2006) reported that there existed three distinct fouling stages during a
mature fouling process in an MBR in the following three sequential
stages: 1) conditioning fouling stage due to fast deposition of microbial
products residue and initial pore blockage; 2) a slow fouling stage
resulting from gradual cake formation, biofilm growth and further pore
blockage; and 3) a transmembrane pressure (TMP) jump stage because
of rapid accumulation of organics and microbial products onto and into
the mature cake layer. Some studies concluded that from the initial
conditioning fouling to the later mature cake layer, fouling formation
was positively correlated with the content of dissolved organic matters
(DOMs) from microbial products (i.e., polysaccharides and proteins)
(Guo et al., 2020; Yao et al., 2010). Further, a recent study reported that
the VMBR could reduce the DOMs in the mixed liquor compared to the
ASMBR, which might help to better mitigate membrane fouling at the
initial stage of TMP rise (Wang et al., 2021). Taken together, these
studies highlighted the need to systematically investigate and charac­
terize the DOMs in the foulant layer during the different fouling stages
between the VMBR and ASMBR. Tracing the fouling constituents and
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Water Research 212 (2022) 118098
their causes during each fouling stage between the two MBRs will be
helpful to investigate the underlying fouling mechanisms and weigh the
pros and cons of the air sparging or membrane vibration in MBRs for
future technology improvement.
Additionally, most of the aforementioned studies on exploring
fouling mechanisms of MBRs remained narrow because of the use of
makeup wastewaters (MWW). In fact, a recent study reported that real
DWW had 5.5 times more proteins and 11 times more polysaccharides
than MWW (Banti et al., 2020). The substantial differences in water
matrices between real DWW and MWW may cause significant variations
in fouling formation. To the best of our knowledge, fouling development
at different fouling stages has not been comprehensively understood in
MBR during real DWW treatment so far. Particularly, there exist
research gaps on how the fouling occurs, behaves and develops between
the VMBR and the commonly applied ASMBR when treating real DWW.
To fill the knowledge gaps, this study comprehensively investigated
the fouling control, fouling development characteristics and fouling
sources across three fouling stages (i.e., 0–10 kPa, 10–20 kPa and 20–30
kPa) between the novel VMBR and conventional ASMBR for real DWW
treatment over a long period (215 days) of operation. The specific ob­
jectives are as follows: (1) effects of different air sparging and vibration
speeds on fouling control in three fouling stages were evaluated by
analysing the TMP changes and fouling rates; (2) fouling behaviours
during each fouling stage of the two MBRs were compared by charac­
terizing the fractioned DOMs in the cake layer; (3) differences in
reversible and irreversible fouling formation among three fouling stages
between the VMBR and ASMBR were examined by the membrane
resistance profiles; and (4) fouling contributors from fractioned mixed
liquor (i.e., colloids, SMP and EPS) between the two MBRs were also
investigated to explore the potential fouling sources.
2. Materials and methods
2.1. MBRs operation and sampling
Two identical flat-sheet MBRs with submerged vibrating and air-
sparging alumina ceramic membrane modules (Meidensha corpora­
tion, Japan) were operated as the VMBR and the ASMBR (Fig. 1),
respectively, at Singapore’s ambient conditions (24~31 ℃ in both
MBRs). The nominal membrane pore size was 0.1 μm with an effective
surface area of 0.008 m2 for each module. In the VMBR, membrane vi­
bration speed was adjusted by a speed controller connected to a recip­
rocating holder fixed with a motor (37GB-520, DC 24 V, 150RPM). The
vibrating amplitude was 25 mm throughout the study. In the ASMBR, an
80-mm diffuser was installed at the bottom of the membrane holder, and
the air sparging rates were controlled by an air flow meter. Each MBR
was operated with 0.98 L of working volume at constant flux of 24 L/
m2•h with 0.2 L-air/min biological aeration at 10-d SRT and 5-h HRT.
Both MBRs were both acclimatized for 30-d (i.e., 3 x SRT) after sludge
seeding from a local DWW water reclamation plant (WRP) in Ulu Pan­
dan, Singapore. They were fed continuously with real DWW from this
plant throughout the experimental study. A 10-min filtration cycle
comprising of 8-min permeation and 2-min relaxation was applied for
both MBRs. Three experimental phases were conducted under three
comparable shear stresses conditions (Table S1) based on the critical
flux test using fresh activated sludge obtained from the local WRP (see
details in SI). The results showed that the critical fluxes between the set
air-sparging rates and vibration speeds (1.5 LPM vs 120 RPM, 1.0 LPM vs
80 RPM, 0.5 LPM vs 40 RPM) were rather similar to each other (Fig. S1).
These results further demonstrated that the shear stresses in each phase
were comparable between the ASMBR and the VMBR (Fig. S1). pH was
maintained at 7.25 ± 0.30 by introducing 0.5 M sodium bicarbonate into
each MBR via metering pumps (DLX-pH-RX Pump, Italy). Dissolved
oxygen (DO) concentration was monitored once a week by a DO meter
(JPSJ-605, Shanghai REX, China). TMP data were logged at 3-min in­
tervals by a digital pressure gage (SMC, ZSE50F) in each MBR. Fouling
C. Wang et al. Water Research 212 (2022) 118098

Fig. 1. A schematic diagram of the two MBRs operated in parallel.

rates were determined by ΔTMP/Δt. min. The organics in the supernatant obtained after the 9000 × g
Influent, permeate and the mixed liquor were sampled every three centrifugation for 10 min and 0.45-µm filtration is considered as EPS.
days; their main characteristics between the two MBRs are listed in
Table S2. Membrane foulants dissolved in 15-mL ultrapure water were 2.2. Membrane resistance determination
collected by gently scraping off the foulant layer using a clean sponge
after each fouling period. Three fouling periods including 0–30 kPa Membrane resistance (R), which is inversely associated with mem­
(CL30), 0–20 kPa (CL20) and 0–10 kPa (CL10) were investigated with at brane permeability, is commonly used to determine the membrane
least 3 cycles during each experimental phase to differentiate three fouling (Jalilvand et al., 2014). According to the Darcy’s law, R (m− 1) is
fouling stages (F1(0–10 kPa), F2(10–20 kPa), F3(20–30 kPa)) as illus­ given by Eq. (1):
trated in Fig. 2a. The data (i.e., DOMs) in F2 of each fouling cycle was
calculated by deducting the results in F1 (CL10) from the corresponding R=
ΔP
(1)
value during 0–20 kPa (CL20) (F2 = CL20 - CL10). The result in F3 was μJ
calculated by deducting the data during 0–20 kPa from the value during
0–30 kPa (CL30) (F3 = CL30 - CL20). Ex-situ chemical cleaning was where ΔP represents the TMP increment (kPa); μ represents the
performed after removing the foulant by soaking the membrane into permeate viscosity (8.90 × 10− 4 Pa•s at 25 ◦ C) and J represents the flux
0.5% citric acid and 0.5% sodium hypochlorite for over 12 h, sequen­ (24 L•m− 2•h− 1). The total filtration resistance (Rt) can be divided into
tially. After sample collection, 5-mL mixed liquor and foulant samples three components: intrinsic membrane resistance (Rm), reversible cake
were used for suspended solids (SS) and volatile suspended solids (VSS) layer resistance (Rr) and irreversible pore blockage resistance (Rir) as
analysis according to the APHA Standard Methods (APHA, 2005). The follows:
method of EPS extraction from the mixed liquor and foulant solution P0
was adopted from Huang et al. (2011) and Yao et al. (2020) as detailed Rm = (2)
μJ
in Fig. 2b. First, supernatant was obtained after 9000 × g centrifugation
for 10 min and filtered from a 1-µm filter (MCE, Pall Corporation), then Pt
Rt = (3)
the further filtered supernatant using a 0.45-µm filter (MCE, Pall Cor­ μJ
poration) was kept as SMP. The content of colloidal organics was
determined by deducting the organics content within SMP from the Rm+ir =
Pi
(4)
corresponding supernatant. Next, the pelleted biomass was resuspended μJ
to the original volume using ultrapure water and heated at 80 ◦ C for 10

Fig. 2. Experimental design for differentiating the fouling stages from different fouling periods (a) and fractioning mixed liquor and cake layer solution (b).

3
C. Wang et al. Water Research 212 (2022) 118098

Rr = Rt − Rm+ir (5) Germany) and three-dimensional excitation emission matrices (EEM)

Rir = Rm+ir − Rm (6)
where P0 is the TMP increase measured by a virgin membrane after 15-
min continuous filtration using Milli-Q water; Pt is the TMP rise obtained
with a fouled membrane after same filtration test; and Pm+ir is the TMP
increase determined after removing the cake layer of the fouled
membrane.
using fluorescence spectrophotometer (Varian Gary Eclipse, Agilent).
Dilution of the samples from the two MBRs were conducted identically
before analysis. In this study, p-value < 0.05 represents statistical sig­
nificance using ANOVA analysis.
3. Results and discussion
3.1. TMP profile and fouling rates

2.3. DOMs characterization and other analyses
Fractioned DOMs in the supernatant, SMP and EPS of the mixed li­
quor and foulant solutions of the two MBRs were characterized by a
liquid chromatography organic carbon detector (LC–OCD) (Dr. Huber,
Under constant flux condition, membrane fouling may be presented
by the increases in TMP with operating time. A quasi-exponential
growth curve, which has been widely acknowledged for decades
(Judd and Judd, 2011; Maqbool et al., 2014), was observed in the TMP
profiles of both MBRs over the high-, middle- and low-shear phases as

Fig. 3. TMP profiles (a) and fouling rates (b) of the two MBRs. (F1 represents the initial fouling rates during 0–10 kPa (10 kPa/Δt1); F2 represents the middle-staged
fouling rates during 10–20 kPa (10 kPa/Δt2); F3 represents the final-staged fouling rates during 20–30 kPa (10 kPa/Δt3); Ft represents the total fouling rates during
0–30 kPa (30 kPa/Δti)).

4
C. Wang et al.
Phase 1, 2 and 3, respectively (Fig. 3a). As the vibration speed reduced
from Phase1 to Phase 3 in the VMBR, the fouling periods from 0 to 30
kPa decreased from 12.99 ± 0.45 d to 7.42 ± 0.69 d and 3.04 ± 0.46 d,
respectively. In the ASMBR, as air-sparging intensity decreased from
Phase1 to Phase 3, the fouling periods from 0 to 30 kPa were reduced
from 3.58 ± 1.28 d to 1.82 ± 0.64 d and 0.71 ± 0.25 d, correspondingly.
Results showed that higher shear stress enhanced by both membrane
vibration and air sparging could mitigate membrane fouling and extend
the fouling periods. The VMBR displayed 70% longer fouling periods
than the ASMBR in all three phases, demonstrating higher effectiveness
in fouling control. A careful look at the TMP profiles indicated that there
were three distinct fouling stages in the entire fouling period, including a
first slow TMP rise stage from 0 to 10 kPa (F1), then a sharp increasing
stage from 10 kPa to 20 kPa (F2) and subsequently a TMP jump stage
from 20 kPa to 30 kPa (F3). Comparison between the two MBRs in
Fig. 3a showed that the VMBR achieved longer duration for all the three
fouling stages (F1, F2 and F3) than the ASMBR, signifying that vibrating
membrane was more effective in retarding the fouling formation in each
fouling stage than air sparging.
Fouling rates (ΔTMP/Δt) in Fig. 3b further showed that total fouling
rates (Ft) and fouling rates each in F1, F2 and F3 were markedly
increased in both MBRs with the decrease in shear stress from Phase 1 to
Phase 3. This indicated that higher shear stress enhanced by air sparging
or membrane vibration could extend the fouling periods in all fouling
stages, particularly in F1, thus retarding the fouling formation. This
implied that F1 might play a crucial role in membrane fouling formation,
which was attributed to a combination of floc deposition and concen­
tration polarization that could be restricted by enhanced shear stress
because hydrodynamic shear could increase the back diffusion of
Fig. 4. Concentrations of fractioned organics (a), DOC of SMPCL (b), EPSCL (c) and VSS (d) of the cake layer in the two MBRs during the three phases.
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Water Research 212 (2022) 118098
particles along the membrane surface (Bérubé, 2020; Delgado et al.,
2008; Menniti et al., 2009). The VMBR showed 61.6% ~ 74.3%, 70.5%
~ 83.8%, 69.4% ~ 85.1% lower in fouling rates for F1, F2 and F3,
respectively, than the ASMBR over the three phases (p < 0.01), indi­
cating that membrane vibration could more effectively control each
fouling stage than air sparging. From the initial fouling (F1) to the final
fouling stage (F3), fouling rates in each fouling stage of both MBRs
presented increasing trends, which were likely attributed to accelerated
foulant formation for higher membrane resistance along with fouling
maturation (Le-Clech et al., 2006; Wang et al., 2014). Furthermore, the
fouling rates in the ASMBR increased more significantly from F1 to F3
than those in the VMBR as shown in Fig. 3b, demonstrating that mem­
brane vibration caused a delay in the TMP rise to alleviate membrane
fouling more effectively. Overall, the VMBR achieved better fouling
control not only in all three phases but also in each fouling stage with
lower fouling rates compared to the ASMBR. Combined analyses of TMP
profiles and fouling rates in different fouling stages would provide
mechanistic insights into better understanding foulingdevelopment and
mitigation, which can also help assess the effectiveness of different
fouling control strategies in MBRs.
3.2. Fouling characteristics
3.2.1. Fractioned organics
Fouling mitigation is highly related to the reduction of the organic
compounds within the cake layer (CL) (Iorhemen et al., 2016; Wang
et al., 2014, 2009a). The fractioned organics (i.e., SMPCL, EPSCL and
colloidCL), as the main substances of cake layer (Wang et al., 2009a),
were monitored during the three phases of this study to explore the
C. Wang et al.
intrinsic fouling characteristics in the two MBRs. As illustrated in Fig. 4,
the organics concentrations of colloidCL in the fouled membrane (Ft) of
the ASMBR were 192.58 ± 42.76, 204.96 ± 45.51 and 225.80 ± 50.13
mg/m2 in Phase 1, 2 and 3, respectively, which were significantly higher
than those of the VMBR with values of 50.60 ± 4.39, 52.32 ± 7.51 and
80.80 ± 10.42 mg/m2 accordingly (p < 0.01). The SMPCL in the Ft of the
ASMBR had organic concentrations of 233.27 ± 38.97, 248.28 ± 41.48
and 273.51 ± 45.69 mg/m2 in Phase 1, 2 and 3, respectively, which
were also much higher than those of the VMBR with values of 66.11 ±
3.64, 68.34 ± 7.76 and 105.54 ± 13.81 mg/m2 correspondingly (p <
0.01). The results demonstrated that membrane vibration was effica­
cious in minimizing the various proportions of organics on the mem­
brane surface, while air sparging was less effective in alleviating the
cake layer formation gelated by colloids and DOMs (Hong et al., 2014),
which might be because the shear enhancement on the full membrane
surface from air sparging was not as even as that of membrane vibration.
These results explained that the fouled cake layer of the VMBR was
comparatively thinner and more compressible than the cake layer of the
ASMBR as illustrated in the supplementary materials (Figs. S2 & S3).
During the different shear stress phases, concentrations of the total or­
ganics in the entire cake layer increased significantly as the shear
stresses were decreased from Phase 1 to Phase 3 in the two MBRs (p <
0.01). The results demonstrated that higher shear stress would reduce
the organics attached to the membrane surface and thus control the
membrane fouling (Delgado et al., 2008). Enhancing vibration speed (i.
e., over 80 RPM) in the VMBR could more effectively reduce colloidCL
and SMPCL attached to the membrane surface than increasing aeration
intensity. Besides, the average concentrations of organics within the
EPSCL bound to the cake layer of the ASMBR were 33.38 ± 4.59, 39.14 ±
5.38 and 43.36 ± 5.97 mg/m2 in Phase 1, 2 and 3, respectively, which
were a bit higher than those in the VMBR with mean values of 31.82 ±
3.71, 33.03 ± 5.77 and 37.08 ± 9.52 mg/m2, accordingly (Fig. 4a). The
result might be attributed to the difference in the biomass concentra­
tions (Fig. 4d) between the two MBRs under similar EPS/biomass ratios
(i.e., ~20 mgDOC/gVSS) (Table S3). In contrast to the EPSCL, it was
evident that the colloidCL and the SMPCL were the main contributors to
membrane fouling (Banti et al., 2020), accounting for over 78.5% and
92.0% of the total organics in the fouled membrane in the VMBR and
ASMBR, respectively. The EPSCL contributed much less organics to cake
layer formation in the two MBRs probably owing to that shear stress
enhancement could detach the biomass away from the membrane sur­
face (Fig. S2) (Bérubé, 2020; Menniti et al., 2009). The VSS concentra­
tions in the cake layer were less than 2.0 g/m2 throughout the three
phases (Fig. 4d), leading to lower concentrations of EPSCL.
Regarding the different fouling stages in Figs. 4a-4c, the content of
colloidCL and SMPCL increased while the EPSCL concentrations decreased
from F1 to F3 in both MBRs, indicating that SMPCL and colloidCL in the
subsequent matured fouling stages could impart accelerated organics
accumulation on the cake layer, while the EPSCL bound to biomass
declined from F1 to F3 due to less biomass attached to the membrane
surface within the shorter time (Fig. 4d). This might be because the
deposition of biomass floc could be substantially restricted under hy­
drodynamic condition induced by air sparging or membrane vibration,
while the adhesion of colloids and dissolved organics onto the mem­
brane surface/fouling layer could not be easily limited due to their non-
settable characteristics (Rosenberger et al., 2006). Compared to the
ASMBR, the organic contents within of the colloidCL and SMPCL in the
three fouling stages of the VMBR significantly reduced by 69.3 ± 4.73%,
especially in F1, indicating that membrane vibration was more effective
to mitigate the initial fouling than air sparging, which was accordingly
illustrated by the TMP profiles in Section 3.1. In the different pro­
portions of organics, DOMs were considered as the dominant com­
pounds to form cake layer and pore blockage reported by Guo et al.
(2020) and Yao et al. (2010). Given that colloids in cake layer were
micro-sized particles ranging from 0.45 μm to 1 μm, they were hardly
presented as dissolved organics (Yao et al., 2020). This study thereby
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Water Research 212 (2022) 118098
further characterized the DOC fractions (i.e., biopolymer and
low-molecular-weight compounds (LMWs)) in the SMPCL and the EPSCL
between the two MBRs during the three phases to explore the underlying
fouling mechanisms (Figs. 4b and 4c). From Phase 1 to Phase 3, the
average DOC concentrations in the cake layer increased in both MBRs,
indicating that shear stress enhancement reduced the accumulation of
DOMs along the membrane surface and thus mitigated fouling.
Compared to the ASMBR, lower DOC concentrations with less
biopolymer and LMWs content were presented in the cake layer of the
VMBR over the three phases (p < 0.01), demonstrating better restriction
of organics deposition in the cake layer by membrane vibration. In the
VMBR, the biopolymer concentrations within the cake layer showed a
decrease of 45.7% ~ 71.7% in the SMPCL and 32.6% ~ 54.0% in the
EPSCL of those in the ASMBR. Owing to the fact that the biopolymers (i.
e., polysaccharides, proteins and aminosugars) ranging from 20 kDa to
0.45 um are the main DOMs driving membrane fouling in MBRs (Meng
et al., 2011; Rosenberger et al., 2006; Yao et al., 2020), lower bio­
polymers content in the cake layer of the VMBR suggested that mem­
brane vibration could more effectively reduce the fouling constituents to
show a lower fouling propensity than air sparging.
A further investigation into the different fouling stages between the
two MBRs found that the SMPCL concentrations increased gradually
from F1 to F3 (Fig. 4b), while the EPSCL showed the opposite trends
(Fig. 4c). These results specified that SMPCL, as the main DOMs in the
cake layer, could be rapidly accumulated along with fouling develop­
ment (Yao et al., 2020). EPSCL bound to the biomass in the cake layer
was gradually reduced from F1 to F3 as biomass concentrations declined
as shown in Fig. 4d with the shorter fouling periods. A closer look at the
DOMs in the cake layer during all three fouling stages revealed that the
VMBR showed remarkably lower concentrations of biopolymers and
LMWs in the SMPCL and the EPSCL compared to the ASMBR (p < 0.01)
(Figs. 4b and 4c). The significant reductions of DOC validated that
membrane vibration could restrict the fouling development from the
initial fouling stage to the subsequent fouling maturation. Overall, the
VMBR exhibited better practicability in mitigating the organic deposi­
tion onto and into the membrane surface and thus reducing the key
foulant constituents (i.e., colloids and SMP). Significant reduction of the
biopolymer content in all three fouling stages of the VMBR explained
higher effectiveness in fouling control.
3.2.2. PS and PN
It is known that the two dominant components of DOMs in the fou­
lant layer are polysaccharides (PS) and proteins (PN). Further analyses
of PS and PN in the SMPCL and EPSCL were conducted in this study
(Fig. 5). Evidently, PN in the SMPCL and the EPSCL had higher content
during all fouling stages than PS in both MBRs. Meanwhile, from Phase 1
to Phase 3, the PN concentrations within the SMPCL and the EPSCL
increased significantly as the shear stress decreased (p < 0.01). Instead,
no significant changes were found in the PS concentrations of the cake
layer over the three phases (p > 0.05). Such results suggested that PN
might play a more critical part in fouling formation than PS despite both
contributing to cake layer formation, which was consistent with the
previous studies (Ng and Ng, 2010). Meanwhile, significant reduction of
the PN content in the VMBR was observed in the SMPCL compared to the
ASMBR during the three phases (p < 0.01), showing that membrane
vibration worked better on fouling control.
A further investigation of the different fouling stages shows that the
PS and PN concentrations in the SMPCL of both MBRs increased from F1
to F3 (Fig. 5a), especially from F2 to F3 (p < 0.01). The results indicated
that PS and PN would be speedily accumulated in the SMPCL after
fouling maturation (Banti et al., 2020; Yao et al., 2010). As for the EPSCL
in the two MBRs, a downward trend from F1 to F3 was observed in
Fig. 5b, which might be attributed to less organics bound to the biomass
in the limited time, displaying similar trends in the previous DOC sec­
tion. In comparison to the ASMBR, we have noticed that the VMBR
reduced more PS and PN in F1 and F2 during the three phases (p <
C. Wang et al.
Fig. 5. Concentrations of polysaccharides and proteins within SMPCL (a) and EPSCL (b) of the cake layer in the two MBRs during the three phases.
0.01). Retardation of the early fouling stages (F1 and F2) was critical to
mitigate membrane fouling as mentioned in Section 3.1. These results
thereby demonstrated that reduced PS and PN concentrations in the
cake layer of the VMBR, especially in F1 and F2, would result in less
membrane fouling and hence achieve better fouling control.
3.2.3. EEM spectra
To further investigate the similarities and differences of DOMs
characteristics in SMPCL and EPSCL among different fouling periods
(CL10, CL20 and CL30) between the two MBRs, three-dimensional EEM
spectra was performed to trackthe root cause of membrane fouling
(Wang et al., 2009a; Yu et al., 2019). All fluorescence peaks afflicted to
the five regions were located at Ex/Em of 200–250/280–330 nm (Region
I), Ex/Em of 200~250/330~380 nm (Region II), Ex/Em of
200–250/380–545 nm (Region III), Ex/Em of 250–280/230–380 nm
(Region IV) and Ex/Em of 280–520/380–545 nm (Region V), which are
related to the aromatic protein I, aromatic protein II, fulvic acid-like
substances, soluble microbial by-products and humic acid-like organic
compounds, respectively (Chen et al., 2003). Fig. 6 shows that aromatic
protein (Region II) and soluble microbial by-products (Regions IV)
dominated among fluorescent organic matters in the SMPCL and EPSCL
from both MBRs. Results indicated that aromatic protein and soluble
microbial by-products were the two major DOMs for fouling formation,
as reported by Kimura et al. (2005). From Phase 1 to Phase 3, the
fluorescent intensities of Regions II and IV became stronger in the SMPCL
and the EPSCL as the shear stress was decreased, indicating that
increasing air sparging or vibration speed would restrict the attachment
of organics to membrane surface and thereby promote fouling mitiga­
tion. Besides, intensities of Regions II & IV in the EPSCL spectra (Fig. 6b)
were much weaker than those of the SMPCL (Fig. 6b) during the three
phases, demonstrating that SMPCL was the major contributor of DOC to
membrane fouling, which was consistent with the previous results in
Section 3.2.1.
In comparison to the ASMBR, the VMBR presented much lower
concentrations of aromatic protein and soluble microbial by-products in
the SMPCL and the EPSCL spectra in the three phases, corresponding to
lower concentrations of PS and PN as reported in the Section 3.2.2.
These results revealed that membrane vibration might better control the
contributions of aromatic protein and soluble microbial by-products to
form cake layer than air sparging. A detailed look at the different fouling
periods in Fig. 6 indicated that in the initial fouling period (CL10), the
main foulant constituents were aromatic protein; then gradual increases
of aromatic protein and soluble microbial by-products were presented in
the mature foulants from CL20 to CL30. Meanwhile, Region IV (soluble
microbial by-products) had much weaker intensities than Region II
(aromatic protein) among the SMPCL and the EPSCL spectra, indicating
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Water Research 212 (2022) 118098
that the DOMs in the foulant of both MBRs were presented with the
following order: aromatic protein > soluble microbial by-products >
others. Compared to the ASMBR, the fluorescent intensities in Regions II
and IV were evidently lower in the VMBR in the CL10, probably
explaining the cause of delaying the early TMP rise by membrane vi­
bration. Overall, membrane vibration exerted more positive impacts
than air sparging in reducing the fouling constituents and thereby con­
trolling fouling formation.
3.3. Fouling resistance
For better understanding the fouling mechanisms in the two MBRs,
the membrane fouling resistance was also analysed during the three
fouling stages under different phases (Jalilvand et al., 2014). The total
fouled membrane resistance (Rt) is composed of intrinsic membrane
resistance (Rm), reversible cake resistance (Rr) and irreversible pore
blockage resistance (Rir). The Rm of virgin ceramic membranes was
tested by Milli-Q water before each running cycle in this study. During
the fouling development, the Rm is assumed as constant because iden­
tical ceramic membrane modules were used in each cycle under the
same operating condition. The average Rm was 1.80 ± 0.08 (× 1011) m −
1
as detailed in Table S4. The changes of membrane fouling resistance in
the two MBRs thereby were identified by the differences in Rr and Rir. As
elucidated in Fig. 7, the Rr in the ASMBR were 38.53 ± 0.24, 40.29 ±
0.24 and 42.31± 0.31 (× 1011) m − 1 with the average percentages of
84.89%, 85.96% and 86.75% in the Rt in Phase 1, 2 and 3, respectively,
which were much higher than those of the VMBR with mean values of
31.28 ± 0.16, 32.23 ± 0.16 and 38.03 ± 0.24 (× 1011) m − 1 or mean
percentages of 84.34%, 85.20% and 88.05% in the Rt, respectively. The
mean values of Rir in the ASMBR were 5.06 ± 0.16, 4.78 ± 0.16 and 4.66
± 0.24 (× 1011) m − 1 in Phase 1, 2 and 3, respectively, which were also
relatively higher than those of the VMBR with average values of 4.01 ±
0.16, 3.80 ± 0.16 and 3.36 ± 0.24 (× 1011) m − 1, correspondingly.
These results indicated that reversible cake layer fouling dominated the
total membrane fouling in both MBRs (Tsuyuhara et al., 2010; Wang
et al., 2020), and higher shear by increasing air sparging or vibration
speeds would minimize the cake layer resistance. In comparison to the
VMBR, the ASMBR presented higher reversible and irreversible fouling
resistance (p < 0.05) likely due to more colloid and SMP accumulated in
its cake layer as reported in Section 3.2. Moreover, more serious irre­
versible fouling in the fouled membrane of the ASMBR was also a result
of severe pore blockage as high air sparging intensity induced more
organics and small-sized particles (Wang et al., 2021).
During each fouling stage (F1, F2, F3), cake layer resistance (Rr)
increased from F1 to F2 to F3 due to accumulated organics (i.e., colloid
and SMP) onto the membrane surface. Whereas irreversible resistance
C. Wang et al.
Fig. 6. Averaged EEM contour maps of SMPCL (a) and EPSCL (b) in the cake layer of the two MBRs during the three phases. (H, M, L stands for the high-shear, middle-
shear and low-shear phase in Phase 1, 2 and 3, respectively. AS signifies ASMBR; V signifies VMBR.).
(Rir) was initially increased from F1 to F2 and then decreased from F2 to
F3, and Rir in the first two fouling stages (F1+F2) was more than 74.6%
and 82.2% of the total irreversible resistance (F1+F2+F3) in the VMBR
and the ASMBR, respectively. The results showed that pore blockage
mainly occurred in the early fouling stages (F1+F2) because of the initial
pore constriction to pore blocking (Le-Clech et al., 2006). In comparison,
significant reduction of irreversible fouling resistance in the early two
fouling stages (F1 + F2) and reversible fouling resistance in all three
fouling stages was observed in the VMBR compared to the ASMBR (p <
0.01), demonstrating that membrane vibration would help alleviate
both reversible and irreversible fouling during the entire fouling pro­
cess. Taken together, these results suggest that vibrating membrane
technology may be an effective alternative to the conventional air
sparging for simultaneous reversible and irreversible fouling control in
MBRs.
8
Water Research 212 (2022) 118098
3.4. Fouling sources
3.4.1. Fractioned organics in the mixed liquor
Generally, cake layer formation and pore blockage in MBRs are
resulted from the organics in the mixed liquor (Díaz et al., 2016; Pan
et al., 2010). The fractioned organic matters in the mixed liquor (i.e.,
colloid, SMP and EPS) between the two MBRs were investigated in this
study to analyze the fouling causes (Fig. 8a). In the ASMBR, the average
organics concentrations of SMP in the mixed liquor (SMPML) were 23.85,
23.12, 23.00 mg/L in Phase 1, 2 and 3, respectively; the mean organic
concentrations of EPS in the mixed liquor (EPSML) were 87.54, 86.11
and 84.20 mg/L, respectively; while the average organic concentrations
of colloid in the mixed liquor (colloidML) were 1.58, 0.69 and 0.67 mg/L,
correspondingly. As for the VMBR, the average organic concentrations
of SMPML were 10.81, 12.21, 18.94 mg/L in Phase 1, 2 and 3, respec­
tively; the mean organic concentrations of EPSML were 61.12, 63.02 and
77.17 mg/L, respectively; while the average organic concentrations of
C. Wang et al.
Fig. 7. The membrane resistances of the two MBRs during the three phases.
colloidML were 0.15, 0.16 and 0.38 mg/L correspondingly. The EPSML
presented much higher concentrations than the SMPML and the colloidML
in both MBRs, implying that EPSML from the mixed liquor might
contribute the most organics to membrane fouling formation (Wang
et al., 2009b). Given that the biomass concentrations between the two
MBRs (Table S2) were rather similar, the higher organic contents in the
colloidML, the SMPML and the EPSML (p < 0.01) were found in the
ASMBR compared with the VMBR, indicating that strong air sparging in
the ASMBR might introduce high environmental disruption to biomass
and release more organics into the mixed liquor, as reported by Meng
et al. (2008) and Menniti et al. (2009). Instead, membrane vibration did
not disrupt the biomass floc as strongly as air sparging and would not
impact the organic release on account of only small interference be­
tween biomass and vibrating membrane. Higher vibrating speed with
enough oxygen transfer (Table S2) in the VMBR would help reduce the
organic production in Phase 1 and 2, while low vibrating speed in Phase
3 might generate less hydrodynamic turbulence for mixture and thereby
induce some low-DO zones in the corner to release more microbial
products (Kim et al., 2006; Wang et al., 2021). Reduced organics release
from the mixed liquor in the VMBR may help explain the superior per­
formance of lower organics concentrations in the effluent (Table S2).
More analyses of DOC in Figs. 8b and 8c clarified that the VMBR
presented much lower biopolymer content in the SMPML and the EPSML
than the ASMBR, reducing fouling constituents for cake layer formation.
Meanwhile, it was clear that the EPSML contained relatively higher
concentrations of biopolymers than the SMPML in both MBRs, indicating
that the EPSML posed a greater potential to fouling formation than the
SMPML in MBRs (Wang et al., 2009b). Significant reduction in the EPSML
of the VMBR in contrast to the ASMBR showed less fouling propensity,
particularly in Phases 1 and 2. These results revealed that higher
Fig. 8. Concentrations of fractioned organics (a), DOC of SMP (b) and EPS (c) of the mixed liquor in the two MBRs during the three phases.
9
Water Research 212 (2022) 118098
membrane vibration (i.e., >80 RPM) could not only enhance the shear
stress along the membrane surface to detach undesired particles, but
also restrict the organic release into the mixed liquor compared to air
sparging, showing better fouling mitigation.
3.4.2. PS and PN in SMPML and EPSML
The variations of polysaccharides (PS) and proteins (PN) within the
SMPML and the EPSML under the three phases are depicted in Fig. 9 to
assess the fouling sources between the VMBR and the ASMBR. The re­
sults showed that the ASMBR had higher concentrations of PS and PN in
the SMPML and the EPSML than the VMBR, significantly in Phases 1 and 2
(p < 0.01), further indicating that higher air sparging intensity might
impact the biomass stability and cause more organic release as
mentioned in Section 3.4.1. The EPSML with higher PS and PN content
contributed more biopolymers for fouling formation than the SMPML
(Wang et al., 2009b). Moreover, the PN concentrations were much
higher than the PS in both the SMPML and the EPSML, specifying that PN
was the key organics in the mixed liquor (Ng and Ng, 2010). As reported
in Section 3.2.2, PN played a more critical role in fouling formation than
PS. Significant reduction of PN in the SMPML and the EPSML of the VMBR
during Phases 1 and 2 compared to the ASMBR (p < 0.01) would help
explain superior fouling mitigation.
3.4.3. EEM spectra of SMPML and EPSML
Further, three-dimensional EEM spectra was performed to under­
stand the DOM characteristics of the mixed liquor between the two
MBRs (Wang et al., 2009a; Yu et al., 2019). Fig. 10 shows that the main
fluorescence peaks of SMPML dominated in Regions II, III, IV & V. Among
these regions, organics in Regions II and III were the major DOMs in the
SMPML of both MBRs, belonging to aromatic protein II and fulvic
acid-like substances. In the EPSML of the mixed liquor, strong intensities
were observed in Regions II & IV linked to aromatic protein and soluble
microbial by-products, corresponding to the main fluorescent com­
pounds in the cake layer (Wang et al., 2009a). The results confirmed that
EPSML in the mixed liquor acted a more paramount role in fouling for­
mation. Aromatic protein and soluble microbial by-products in the
EPSML were the key contributors to fouling formation.
In contrast, the fluorescent intensities in Region II and IV of both
SMPML and EPSML spectra became stronger in the VMBR while weaker in
the ASMBR from Phase 1 to Phase 3. The results demonstrated that
enhancing membrane vibration was effective in organics reduction
while increasing air sparging might induce more organics, which were
consistent with the previous results of organics in Section 4.1 & 4.2.
Higher vibrating speed (i.e., >80 RPM) in the VMBR would provide
better oxygen transfer (Table S2) and help reduce the production of
aromatic protein and soluble microbial by-products, while low vibrating
speed (i.e., 40 RPM) in Phase 3 with less hydrodynamic agitation might
create some low-DO zones in the corner to release more proteins and
soluble microbial products (Kim et al., 2006; Wang et al., 2021). As for
air sparging, higher aeration intensities might disrupt the biomass when
scouring the mixed liquor with high shear, and thus produce more
C. Wang et al. Water Research 212 (2022) 118098

Fig. 9. Concentrations of polysaccharides and proteins within SMPML (a) and EPSML (b) of the mixed liquor in the two MBRs during the three phases.

Fig. 10. Averaged EEM contour maps of SMP (a) and EPS (b) in the two MBRs during the three phases.

proteins and microbial products (Padmasiri et al., 2007). Overall, the
VMBR under higher shear phase (i.e., >80 RPM) presented much lower
concentrations of aromatic proteins and soluble microbial by-products
in the SMPML and the EPSML compared to the ASMBR, showing higher
effectiveness in reducing fouling sources.
4. Conclusions
From the perspective of fouling development, this study compre­
hensively investigated fouling control, fouling characteristics and
fouling sources across three fouling stages between the novel vibrating
MBR and common air-sparging MBR during long-term real DWW
treatment. Results demonstrated that vibrating membrane technology
was effective in controlling fouling constituents and its sources in the
early fouling stages, making this a competitive strategy with the po­
tential to replace conventional air scouring for fouling mitigation in
MBR treating real wastewater. The key findings and implications are:
1) The VMBR achieved 70% lower fouling rates compared to the
ASMBR during each fouling stage. Higher vibration speed (i.e., 120
RPM) achieved lower fouling rates (i.e., 2.3 kPa/d) because of effective
retardation of the three fouling development stages.
2) Reversible cake layer fouling contributed over 84% of the total
fouling resistance in both the MBRs, which intensified from F1 to F3.
While irreversible fouling (i.e., pore blockage) mainly occurred in the

10
C. Wang et al.
early fouling stages (i.e., F1 and F2).
3) ColloidCL and SMPCL were the two key organic substances in both
cake layers. The VMBR achieved 62.7% reduction in colloidCL and
SMPCL compared to the ASMBR to simultaneously alleviate the revers­
ible and irreversible fouling.
4) The main DOMs in the foulant of both MBRs were found with the
following order: aromatic protein > soluble microbial by-products >
others. Membrane vibration could reduce aromatic proteins and soluble
microbial products of the cake layer during the three fouling stages to
better mitigate membrane fouling compared to air sparging.
5) EPSML contributed more DOMs to cake layer formation than
SMPML from the mixed liquor. Lower concentrations of aromatic pro­
teins and biopolymers in the EPSML of the VMBR led to the reduced
fouling sources for better fouling control compared to the ASMBR.
This study provided novel insights into the membrane fouling
mechanisms and evaluated two different fouling control approaches for
future MBR applications in real wastewater treatment. More in­
vestigations on intermittent vibration modes coupled with backwash in
this novel VMBR for energy-efficient fouling control through pilot- and
full-scale studies are recommended.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgment
The authors would like to thank Ms. Qianxun Yang and Ms. Wenhui
Hu for their help in experimental analysis. The authors also appreciate
the financial support from the NUS Research Scholarship (PVO-SP).
Supplementary materials
Supplementary material associated with this article can be found, in
the online version, at doi:10.1016/j.watres.2022.118098.
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