Chemical Engineering Journal 273 (2015) 223–230

Contents lists available at ScienceDirect

Chemical Engineering Journal

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

Low-voltage electric field applied into MBR for fouling suppression:

Performance and mechanisms
Jiao Zhang, Abdallatif Satti, Xingguo Chen, Kang Xiao 1, Jianyu Sun, Xiaoxu Yan, Peng Liang,
Xiaoyuan Zhang, Xia Huang ⇑
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

h i g h l i g h t s

 Intermittent low voltage electric field depressed fouling in membrane bioreactor.

 Electrolyzed iron reduced foulant by reacting with soluble microbial product.
 Electrophoresis might make fouling layers loose rather than remove foulant.
 Irreversible and overall fouling were reduced by above two joint effects.

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

Article history: A low-voltage electro-membrane bioreactor (e-MBR) for fouling alleviation was designed using stainless
Received 27 November 2014 steel anodes and a membrane module containing titanium cathodes (Fe-MBR). The electric field was
Received in revised form 23 February 2015 applied intermittently once the suction pump was stopped. Compared with another e-MBR with titanium
Accepted 10 March 2015
anodes (Ti-MBR) and with one MBR without an electric field, the Fe-MBR had lower transmembrane pres-
Available online 17 March 2015
sure (TMP), less irreversible fouling and higher pollutant removals under an intermittent voltage of
2.72 V and current of 0.1 A. Coagulation was not obvious because no significant changes were observed
Keywords:
in either particle size or zeta potential. The electric field induced backwash was confirmed, by the Ti-
Membrane bioreactor
Electric field force
MBR, to be effective to suppress fouling. The electric field force might prevent the tight precipitation
Electrolyzed iron of foulant on the membrane’s surface and make the fouling layers looser and easier to be removed by
Soluble microbial products aeration. Besides, a strong positive correlation was obtained between fouling indexes and total organic
Transmembrane pressure carbon of soluble microbial products (SMPs), suggesting that the reduction of SMPs in the Fe-MBR could
have resulted in the fouling depression, and was related to the release of iron. Thus, the joint effects of the
electric field force and the release of iron deducted foulant and irreversible fouling, and ultimately less-
ened the overall fouling. The energy consumption estimation showed 10% more electricity was consumed
to make TMP reduce by 30%, indicating the Fe-MBR would be promising in application.
Ó 2015 Elsevier B.V. All rights reserved.

1. Introduction A membrane, in e-MBRs, could be put either outside or inside

Membrane bioreactors (MBRs) have been widely used for
wastewater treatment [1,2], however, membrane fouling is an
essential problem which shortens the membrane’s life and raises
its operational cost. Many methods have been investigated to alle-
viate the fouling in MBRs [3–5] , among which electro-MBRs (e-
MBRs) were researched by applying an electric field into MBRs
[6] as an option.
⇑ Corresponding author. Tel.: +86 10 6277 2324.
E-mail addresses: xiaok02@gmail.com (K. Xiao), xhuang@tsinghua.edu.cn
(X. Huang).
1
Co-corresponding author. Tel.: +86 10 88257606.
the electric field. If it is located outside the electric field, fouling
suppression would be achieved by modification of the mixed
liquor. In this case, iron [7,8] or aluminum [9] was usually used
as the anode from which metal ions would be released when the
electricity was conducted. The electrically released ions would
hydrolyze and form hydrated oxides which act as coagulants.
This effect was illustrated as electro-coagulation [10]. If the mem-
brane is located inside the electric field, the cathode would be
designed to be part of the membrane module [11–13]. Besides
electro-coagulation, electrophoresis is accessible for the fouling
alleviation as well, i.e. negatively charged foulants would move
away from membrane surface due to the electric field force [14].

http://dx.doi.org/10.1016/j.cej.2015.03.044
1385-8947/Ó 2015 Elsevier B.V. All rights reserved.
224 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230
Unlike electro-coagulation, electrophoresis is independent of the
anode material.
However, the electric field would raise the cost of the MBR in
some instances. A lot of electricity would be consumed with an
inactive metal as the anode. Electric field strength up to 50 V/cm
was required for the recovery of flux by electric field with carbon
electrodes [11]. Additionally, the novel conductive membrane
module [13] might generate a high material and processing cost
as well. Moreover, additional and thorough studies are required
to investigate the effects of low voltages on membrane fouling
development as well as foulant components, the relationship
between overall fouling and properties of mixed liquor, and the
distinct mechanisms of fouling reduction in e-MBRs especially
when both electro-coagulation and electrophoresis possibly exist.
Therefore, in this study, aiming at suppressing fouling with low
energy consumption, two e-MBRs were designed and operated
parallel with another conventional MBR, and their performance
in fouling depression was investigated. Both of the e-MBRs were
operated with the same current supply, one of which had stainless
steel anodes (Fe-MBR) and the other had titanium ones (Ti-MBR).
The Fe-MBR was supposed to be the low-voltage e-MBR and
involved the functions of both electric field force and electro-coa-
gulation; while the Ti-MBR was designed mainly to identify the
effectiveness of the electric field force in fouling depression. The
mechanisms of fouling suppression were discussed as well accord-
ing to the changes of the parameters in the mixed liquor.
2. Materials and methods
2.1. Set-up and membrane module
An e-MBR was constructed with an effective volume of 10 L
(Fig.1(a)). A flat sheet of a ceramic membrane (Meiden, Japan) with
a pore size of 0.1 lm and an effective area of 0.035 m2 per side was
submerged in the middle of the reactor. Titanium sticks inserted
into the flat sheet ceramic membrane (Fig.1(b)) were used as cath-
odes, and two pieces of metal mesh, serving as anodes, were placed
35 mm away from the membrane on each side. The e-MBR with
the stainless steel mesh as the anode was named as Fe-MBR, and
the titanium mesh one was named as Ti-MBR. The effective area
of each anode was 0.035 m2. One more MBR with the same size
and arrangement but without an electric field applied was run par-
allel as a control. The flux of each MBR was fixed at 15 L/(m2 h), and
the suction pump for each reactor was operated for 8 min ON and
2 min OFF, and the electric field was applied by a direct current
(DC) supplier as soon as the suction was stopped. For all the experi-
ments, synthetic domestic wastewater was fed as raw wastewater
with the compositions of (in mg/L): glucose (175), starch (139),
peptone (19), urea (32), NH4Cl (153), K2HPO4 (22), MgSO4-7H2O
(66), CaCl2-2H2O (23), NaHCO3 (111), MnSO4 (2.6) and FeSO4
(0.4). The activated sludge mixed liquor used was taken from an
aeration tank of Beixiaohe municipal wastewater treatment plant
located in Beijing. The aeration intensity was 1.0 m3/h to ensure
the concentration of dissolved oxygen above 2.0 mg/L. Trans-mem-
brane pressure (TMP) was automatically recorded as well as the
contemporary temperature.
2.2. Experimental operation
Preliminary experiments with varied electric current and elec-
tric loading duration were conducted to locate the operational
electric field conditions of the Fe-MBR as applying DC for 2 min
with current of 0.1 A (Fig. S1 in supporting material), and the
corresponding voltage was on average 2.72 ± 0.13 V. The Ti-MBR
was operated at the same current with the Fe-MBR, and the voltage
was on average 7.79 ± 0.08 V.
Two series of long runs were conducted to investigate the per-
formance of e-MBRs. First, long-runs were conducted with a clean
membrane module and fresh mixed liquor, and repeated 3 times in
order to investigate the overall fouling reduction and repeatability.
Second, long-runs with the physical washing of the fouled mem-
brane module were operated aiming at observing the irreversible
fouling development. During the experiment, the membrane mod-
ule was taken out when the TMP reached 35 kPa, and then put back
in the reactor after being washed only by tap water to continue
operating. For each reactor, the membrane module was washed
three times.
2.3. Measurement and analysis
Pollutants for both influent and effluent, in terms of chemical
oxygen demand (COD), NH+4-N and total phosphorus (TP), were
measured using standard methods [15], and so were mixed liquor
suspended solids (MLSS) and mixed liquor volatile suspended
solids (MLVSS). The sludge volume index (SVI) was measured to
quantify the settle-ability of the mixed liquor [16]. Particle size
of the mixed liquor was measured as the volume mean diameter
(LS™ 13320/ULM2, Beckman Coulter, USA).
The mixed liquor was centrifuged after being sampled and fil-
tered by a 0.7 lm glass microfiber filter (Grade GF/F, Whatman,
UK) to get the supernatant containing soluble microbial products
(SMPs), of which the Zeta potential was measured by a zeta poten-
tial analyser (Delsa™ Nano C, Beckman Coulter, USA), and the Fe
concentration was measured using IRIS Intrepid II XSP (Thermo,
USA). A heat extraction method was applied to obtain both loosely
bounded extracellular polymeric substances (LB-EPS) and tightly
bounded ones (TB-EPS) [17]. Total organic carbon (TOC) of both
SMP and EPS were measured by the TOC analyser (TOC-VCPH,
Shimadzu, Japan), and so were other contents such as polysaccha-
ride [18], protein and humic substance [19], using D-glucose
(Sigma, USA), bovine serum albumin (BSA) (Sigma, USA) and humic
acid (Fluka, Switzerland) as the standards respectively. Before the
determination of protein, divalent cations were removed by gel-
type cation exchange resins (Amberlite IR-120 Na, Acros
Organics, Belgium) in order to get rid of the interference of calcium
and magnesium [20].
Additionally, the fouling rate was calculated, which was the
slope of TMP over time. The fouling resistance of mixed liquor
and fouling propensity of supernatant were determined as specific
resistance to filtration (SRF) of sludge and supernatant respec-
tively, using a dead-end filtration system [21] at a constant pres-
sure of 10 kPa. The SRF was calculated as
2b  A2  DP
SRF ¼ ð1Þ
lC
where SRF was specific resistance to filtration (m/kg), A was the
effective filtration area (m2), DP was the pressure applied during fil-
tration (Pa), l was the viscosity of filtrate (Pa s), C was the concen-
tration of suspended solid (kg/m3), and b was the slope of filtrate
volume over time versus time (m3/s2).
3. Results and discussion
3.1. Fouling suppression and pollutants removal
3.1.1. TMP evolution
Fouling conditions in both e-MBRs were significantly alleviated
in both two series of long-run, characterized as the lower TMP
observed than that of the control MBR (Fig. 2). In the 3 long-runs
 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230
Fig. 1. Schematic of (a) MBR set ups and (b) membrane module with cathode inserted (1. feed water tank; 2. influent pump; 3. aeration pump; 4. membrane module with
cathode; 5. stainless steel mesh in Fe-MBR and Titanium mesh in Ti-MBR; 6. membrane module with cathode; 7. water level sensor; 8. pressure sensor; 9. effluent pump; 10.
DC supplier; 11. ceramic membrane module; 12. titanium stick; 13. water channel).
with clean membrane module and fresh mixed liquor, at the time
when the control MBR was stopped, the TMPs of Fe-MBR were
25.3%, 40.4% and 31.3% lower than those of the control MBR
respectively, and the TMPs of Ti-MBR were 25.3%, 28.9% and
20.0% lower than those of the control MBR respectively
(Fig. 2(a)), indicating the effectiveness and repeatability for overall
fouling suppression in e-MBR.
In the operation with physical washing, the membrane modules
of e-MBRs were washed less frequently than that of the control
MBR (Fig. 2 (b)), i.e., the e-MBRs had a persistent performance in
repressing TMP evolution. Besides, each time after washing, the
initial TMPs of the e-MBRs were lower, indicating less irreversible
foulant on the membrane surface. After washing the membranes 3
times, the development of irreversible fouling could be drawn as
the lines [22], of which the slope indicated the irreversible fouling
rate. Apparently, the slope in both e-MBRs grew more slowly than
that in the control MBR, i.e. the irreversible fouling grew slower in
the e-MBRs, suggesting that less foulant in the mixed liquor caused
irreversible fouling and/or the foulant layer formed on the mem-
brane surface was easier to remove.
Besides, the TMPs of Fe-MBR were lower than or close to that of
Ti-MBR both in the runs with and without any physical washing
(Fig. 2), indicating that the usage of stainless steel anodes benefited
fouling suppression better than the titanium ones. Compared with
the Ti-MBR which only had an electric field force, the Fe-MBR was
designed to release iron as well. So, the lower TMPs in the Fe-MBR
225
suggested the effectiveness of the expected iron release on fouling
depression.
3.1.2. Effect of exerted electrical field on pollutants removal
Both e-MBRs and control MBR showed COD removal with a
removal rate approximately 95% (Table 1). Enhanced TP removal
was observed in the Fe-MBR (91.7%) compared with that in the
control MBR (46.2%) and Ti-MBR (42.4%). It might be because that
iron ions generated from the stainless steel anode could react with
the phosphorous in the mixed liquor to form insoluble precipitates.
However, both the Fe-MBR and the Ti-MBR had a lower removal
efficiency of NH+4-N (81.9% and 52.4% respectively) than that of
the control MBR (88.9%). This phenomenon was observed as well
in other researches [7,8,13], suggesting the possible inhibition
effect of an electric field on the growth of nitrifying bacteria and/
or the nitrification process in the MBR. The metabolism of nitrify-
ing bacteria in an activated sludge was found to be inhibited when
the applied current density was over 2.5 A/m2 and this inhibition
was attributed to the destruction of bacteria cells with large cur-
rent densities [23]. In this study, the current density was 2.8 A/
m2, which was slightly larger than 2.5 A/m2, so the nitrification
would be inhibited slightly. However, the NH+4-N removal in the
Fe-MBR (81.9%) was slightly lower than that of the control MBR
(88.9%), while the Ti-MBR was much lower (52.4%). Since both
the Fe-MBR and the Ti-MBR were operated at the same current
density and the voltage applied in Fe-MBR was 2.72 V while that
226 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230

Fig. 2. TMP changes of e-MBRs and control MBR in long-run experiments (a) with clean membrane module in each run, and (b) with physical washing (membrane of control
MBR was physically washed at 150 h and 190 h; Ti-MBR at 160 h and 225 h; and Fe-MBR at 170 h and 245 h) at electric current of 0.1 A and loading duration of 2 min/10 min.

Table 1
Pollutant removal efficiencies of MBRs.

Pollutant Influent (mg/L) Control MBR Fe-MBR Ti-MBR

Effluent (mg/L) Removal (%) Effluent (mg/L) Removal (%) Effluent (mg/L) Removal (%)
COD 335 ± 33.1 20.1 ± 4.3 94.0 ± 0.8 16.3 ± 4.0 95.1 ± 1.3 21.4 ± 5.1 93.7 ± 0.1
NH+4-N 28 ± 1.2 3.12 ± 0.4 88.9 ± 1.3 5.08 ± 0.5 81.9 ± 1.1 12.9 ± 0.8 52.4 ± 3.1
TP 4.91 ± 0.4 2.64 ± 0.4 46.2 ± 11.6 0.41 ± 0.12 91.7 ± 3.4 2.72 ± 0.38 42.4 ± 13.4

in Ti-MBR was 7.79 V, the higher voltage of the electric field was
assumed to have a stronger inhibition on nitrification.
3.2. Effect of exerted electrical field on mixed liquor properties
3.2.1. Sludge properties
No significant differences were observed between the e-MBRs
and the control MBR in the aspects of biomass properties
(Table 2). The MLSS concentrations of the Fe-MBR (5790 mg/L)
and the Ti-MBR (5150 mg/L) were changed within 10% compared
with that of the control MBR (5460 mg/L). The VSS/SS ratios of
the 3 MBR’s were close to 80%. Particle size and zeta potential
are regarded as two indicators of coagulation. The particle size
(quantified as the volume mean diameter) of the sludge in the
Ti-MBR (86.2 lm) was larger than that of the other two MBRs,
while the difference between the Fe-MBR (75.0 lm) and the con-
trol MBR (74.2 lm) was negligible; and the absolute value of the
zeta potential was slightly reduced in e-MBRs, making it unclear
whether the coagulation effectively occurred.
Although a reduction of TB-EPS was observed in e-MBRs for TOC
and polysaccharide, the change of LB-EPS was negligible (Table 2).
Since EPS is believed to act as the glue that binds cells together to
form sludge flocs and LB-EPS (as TOC) was observed to have a
negative correlation with bio-flocculation [17], the insignificant
change in EPS was a possible explanation of the negligible change
in particle size and zeta potential.
3.2.2. Supernatant properties
Concentrations of TOC and main organic components of super-
natant were obviously lower in the Fe-MBR than in the control
MBR (Fig. 3(a)), suggesting a reduction of SMP under the electric
field. The TOC in the Fe-MBR was averaging 14.5 mg/L, which
was 18% lower than that in the control MBR (17.7 mg/L).
Polysaccharide, which was believed to be the major foulant [24],
 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230 227

Table 2
Sludge properties of MBRs.

Parameters Control MBR Fe-MBR Ti-MBR

MLSS (mg/L) 5460 ± 77 5790 ± 165 5150 ± 401
MLVSS (mg/L) 4400 ± 14 4540 ± 60 3930 ± 200
VSS/SS (%) 81.8 ± 1.5 78.0 ± 1.5 81.0 ± 4.7
SVI (ml/g) 137.9 ± 44.5 129.5 ± 41.4 142.7 ± 52.0
Volume mean diameter (lm) 74.2 ± 7.2 75.0 ± 4.5 86.2 ± 3.4
Zeta potential (mV) 15.37 ± 2.72 14.73 ± 2.21 14.73 ± 2.22
LB-EPS (mg/g VSS) TOC 3.85 ± 0.34 3.32 ± 0.23 3.72 ± 0.63
Polysacch. 1.56 ± 0.50 1.33 ± 0.10 1.41 ± 0.32
Protein 2.69 ± 0.80 2.42 ± 1.04 3.49 ± 1.56
Humic subs. 2.15 ± 0.65 2.28 ± 0.05 2.95 ± 0.90
TB-EPS (mg/g VSS) TOC 33.20 ± 5.20 25.54 ± 6.12 26.73 ± 7.40
Polysacch. 12.45 ± 2.39 8.98 ± 2.29 9.28 ± 1.19
Protein 10.62 ± 0.23 10.99 ± 0.62 12.19 ± 1.33
Humic subs. 17.84 ± 0.34 15.95 ± 2.18 14.31 ± 4.30

approximately 8 V in the Ti-MBR might stimulate the production

of SMP which was accumulated in the tank without precipitation
by coagulation.

3.3. Mechanisms of membrane fouling depression in e-MBR

3.3.1. Fouling index change of MBRs

Fig. 3. Supernatant contents in terms of (a) organic matter in control MBR and e-
MBRs and (b) the initial and final iron concentration in Fe-MBR.
had a concentration of approximately 13.9 mg/L in the Fe-MBR
compared with that in the control MBR of 16 mg/L. The lower con-
centration indicated less foulant in supernatant, i.e. less potential
to generate membrane fouling. Besides, the quantity of Fe ions in
the Fe-MBR was significantly increased after applying an electric
field (Fig. 3(b)). Since the influent prepared contained negligible
concentrations of Fe, its increase in supernatant should be due to
the release of iron from the stainless steel anodes in the electric
field, which had the potential of forming coagulation in the mixed
liquor.
However, the concentrations of both TOC and polysaccharide in
the Ti-MBR were respectively 32.4% and 23.4% higher than that of
the control MBR (Fig. 3(a)). Compared with Fe-MBR, Ti-MBR had a
higher voltage, and no coagulant ions (such as Fe2+, Al3+) were gen-
erated from the titanium anodes. Thus, the voltage of
As can be seen in Fig. 4, the fouling rates in both e-MBRs were
lower than that of the control one, among which the Fe-MBR had
the lowest (30% lower than control MBR). As to the specific resis-
tance to filtration (SRF) of either mixed liquor or supernatant, the
Fe-MBR had less fouling propensity than the control MBR.
However, the SRF of the mixed liquor in the Ti-MBR
(17.77  1010 m/kg-MLSS) was higher than that of the control
MBR (11.85  1010 m/kg-MLSS), and the SRF of supernatant in Ti-
MBR was twice of that of the control MBR (Fig. 4). Since the 3
MBRs were operated under the same working conditions except
for the electric field, the change of fouling indexes among 3
MBRs should be due to the electric field.
The electric field in the e-MBRs would influence the fouling con-
dition in two different ways. One was the electric field force which
was working on charged particles in the MBR. The other was the
modification of the mixed liquor properties: the potential applied
on the mixed liquor might change the viability of microorganisms
[23,25], and the coagulant-ion released from an active metal anode
(such as Fe, Al) would affect the mixed liquor by coagulation. To
clarify the mechanisms of fouling depression in the e-MBRs in this
study, the titanium mesh anodes in the Ti-MBR were inactive
metal and would not release any coagulant ions, thus the Ti-MBR
was supposed to identify the effectiveness of the electric field force
and modification of the mixed liquor properties under the applied
potential. The stainless steel mesh anodes in the Fe-MBR could
release iron ions under an electric field, i.e. the electric field in
the Fe-MBR would have all the effects on the fouling condition.
The comparison among the 3 MBRs and discussion on the two
designated functions would make it clear what was the main rea-
son for the fouling depression.
3.3.2. Effect from electric field force
The electric field in this study was applied intermittently, and it
was applied as soon as the suction pump was stopped. Thus, the
electric field was supposed to influence the attached particles on
the membrane surface. In the e-MBRs, particles in the mixed liquor
were negatively charged, and when the electric field was applied,
these particles would suffer the repulsive force from the cathodes
in the membrane module and the force would be in the direction
228 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230

Fig. 4. Fouling rate and propensities of control MBR and e-MBRs (SRF refers to specific resistance to filtration, with unit of m/kg-TOC for supernatant and m/kg-MLSS for
mixed liquor).

away from the membrane surface. Thus, this repulsive force from
the electric field would have an effect similar to backwash.
The equivalent backwash flux induced by the electric field is
related to the velocity of the charged particles in the mixed liquor,
and it could be calculated as
Qp
J backwash ¼ ¼ 103  v
A the Faraday’s Law [27,28], and the electro-coagulation was widely
ef
vp ¼ E ð3Þ
l different extents, because of either the release of iron or the poten-
DU I correlation was processed to identify the significance of the mixed
E¼ ¼ ð4Þ
d rA
where Jbackwash is the equivalent backwash flux of the electric field
(L/(m2h)), Qp is the flow rate of water conveying charged particles
(m3/s), A is the effective area of the membrane (m2), vp is the elec-
trophoresis velocity of charged particles (m/s) and is assumed to be
equal to the velocity of water flow under ideal conditions, E is the
electric field strength (V/m), f is the zeta potential of particles (V),
e is the electrolyte permittivity, l is the viscosity of permeate
(Pa s), DU is the voltage applied on the bulk solution (V), d is the
distance between the two electrodes (m), I is the current applied
(A), and r is the conductivity of the bulk solution (S/m) [26].
Since the Ti and Fe had different indigenous potential drops on
the electrodes, it was better to calculate the actual electric field
strength by current.
In this study, the currents of both e-MBRs were fixed at 0.1 A.
Applying the detected conductivity and zeta potential, the elec-
trophoresis velocity in the Fe-MBR and the Ti-MBR were
(4.97 ± 0.08)  107 m/s and (4.94 ± 0.77)  107 m/s, meaning
that the equivalent backwash fluxes were 1.79 ± 0.03 L/(m2 h)
and 1.78 ± 0.29 L/(m2 h) respectively. Compared with the water
flux of 15 L/(m2 h), the equivalent backwash flux provided by the
electric field was approximately 10% of the water flux. Since the
TMP of the Ti-MBR was lower than that of the control one during
the operation (Fig. 2), the electric field induced backwash could
reduce the increasing rate of TMP in the Ti-MBR.
The cake layer and the loosely attached gel layer were supposed
to be removed by shear force from aeration. Compared with aera-
tion intensity, the electric induced backwash flux might have a
negligible effect on the removal of such foulant. However, under
the electric field force, a charged particle on the membrane surface
would have the potential of moving away from the membrane sur-
face, thus the fouling layers would become looser and a tight
attachment would be prevented. Along with aeration, those looser
layers would be removed more easily, and the increase of TMP
would be reduced.
3.3.3. Effect from modification of mixed liquor properties
Mixed liquor properties might be influenced by the electric field
applied to the biomass [25]. Moreover, once the DC was supplied,
iron ions were released from the stainless steel anodes obeying
ð2Þ
accepted as the mechanism and fate of the released iron [7,8,10].
Thus, the mixed liquor properties in the e-MBRs were changed to
tial applied to the mixed liquor (Table 2, Fig. 3, Fig. 4). The pearson
liquor parameters that might affect the fouling rate and SRFs in the
3 MBRs.
It was obtained that SMPs (quantified as TOC) were highly posi-
tively correlated to the fouling rate and the SRF of the mixed liquor
(r > 0, p < 0.05) in both the Fe-MBR and the control MBR, while no
correlations were observed for other properties to fouling rate
(Table 3). Since SMPs were found to be major foulants for mem-
brane fouling [16,29,30] and since the higher TOC in supernatant
was observed to have a higher fouling intensity in MBR [24], the
positive correlations between SMPs and fouling indexes in this
study should be convincing, and SMPs should be one crucial factor
influencing fouling evolution in the Fe-MBR and the control MBR.
The SMPs in the Fe-MBR were observed to be obviously reduced
(Fig. 3), thus the reduction of TOC and polysaccharide of SMPs
would result in the fouling alleviation in the Fe-MBR, which con-
tained less soluble foulant to attach on the membrane and form
a fouling layer.
To be addressed, in the Ti-MBR, the SMP concentration was
higher than the other two MBRs (Fig. 3), which might be attributed
to the high voltage applied to the microorganism which would
stimulate the production of SMPs or break the bacterial cell. In
either way, the SMPs were increased. Considering that SMPs were
the main foulant in the MBR, the increase of SMPs in the Ti-MBR
would result in the significant increase of SRF in both the mixed
liquor and the supernatant (Fig. 4). However, TMP in the Ti-MBR
was lower than that of the control MBR (Fig. 2) and generated a
slower fouling rate (Fig. 4), indicating that the fouling suppression
in the Ti-MBR was attributed to other factors other than the SMP
change. Besides, the mean particle size was increased while the
MLSS concentration was decreased in Ti-MBR (Table 2), which
might also depress the fouling to some extent [16]. Thus the mod-
ification of the mixed liquor properties had a complex effect on
fouling development in the Ti-MBR: the increase of SMPs would
increase fouling, but the increase of mean particle size and the
 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230 229

Table 3
Pearson correlation between mixed liquor properties and fouling indexes.

Mixed liquor properties Fouling rate SRF of mixed liquor SRF of supernatant
Control Fe-MBR Ti-MBR Control Fe-MBR Ti-MBR Control Fe-MBR Ti-MBR
MLSS (mg/L) r 0.150 0.150 0.065 0.220 0.093 0.367 0.134 0.436 0.161
p 0.700 0.701 0.868 0.570 0.799 0.297 0.775 0.280 0.703
Mean particle size (lm) r 0.149 0.409 0.709 0.160 0.243 0.488 0.021 0.156 0.486
p 0.702 0.275 0.114 0.680 0.499 0.152 0.964 0.713 0.222
Zeta potential (mV) r 0.120 0.031 0.028 0.136 0.711 0.672 0.164 0.559 0.030
* *
p 0.778 0.941 0.952 0.749 0.032 0.068 0.725 0.150 0.949
LB-EPS (mg TOC/L) r 0.047 0.139 0.161 0.089 0.954 0.911 0.393 0.412 0.152
* *
p 0.913 0.743 0.704 0.835 0.000 0.001 0.384 0.311 0.720
TB-EPS (mg TOC/L) r 0.068 0.113 0.495 0.122 0.316 0.615 0.039 0.717 0.195
*
p 0.874 0.791 0.212 0.773 0.407 0.078 0.934 0.045 0.644
SMP (mg TOC/L) r 0.600 0.748 0.203 0.982 0.979 0.764 0.600 0.685 0.153
* * * * ⁄
p 0.116 0.033 0.662 0.000 0.000 0.027 0.208 0.133 0.743
*
The significant correlation.

reduction of MLSS concentration would reduce fouling.
Considering the significant increase of SRF in both the mixed liquor
and the supernatant in the Ti-MBR, the modification of the mixed
liquor properties in the Ti-MBR ultimately resulted in worse filter-
ability of the mixed liquor and higher fouling in the gel layer for-
mation, which would increase fouling development. Therefore,
the fouling depression in the Ti-MBR would be mainly due to the
electric field induced backwash.
Additionally, in terms of the reduction of SMPs in the Fe-MBR, it
might be due to the release of iron from the anodes, which could
have reacted with the SMP contents and formed insoluble sub-
stances [28,31,32]. Since the particle size of the mixed liquor was
not significantly affected (Table 2), those insoluble particles might
have been small sizes [28] and were not sufficient to change the
mean particle size of activated sludge flocs. Additionally, although
no significant difference of mean particle size was obtained
between the Fe-MBR and the control MBR (Table 2), the portion
of particles with sizes over 100 lm was slightly larger in the Fe-
MBR than that of the control MBR at the end of the run with physi-
cal washing (Supporting material, Fig. S2), suggesting that the sig-
nificant increase of the flocs’ size in the Fe-MBR might be observed
in the run with longer operation time and with more iron ions
being released from the anode.
Therefore, as shown in Fig. 5, the mechanisms of fouling depres-
sion in the e-MBR were the complex result of reactions at the anode
and electric field force, which had effects on the modification of the
mixed liquor properties and influenced the fouling development. In
the Fe-MBR (as the low-voltage e-MBR), the mechanisms could be
illustrated in two parts (Fig. 5). One was the electric field force
induced backwash, and this effect might prevent tight attachment
of foulant on the membrane surface and loosen the fouling layer
so that it could be removed by aeration easily. The other mecha-
nism would be the iron ions released from the stainless steel anode,
which reacted with organic matter in the supernatant and resulted
in the reduction of TOC and polysaccharide of SMPs. Successively
the foulant on the membrane was reduced, and the filtration resis-
tance of the mixed liquor was lessened as well as the fouling
propensity of the supernatant. Thus, in the Fe-MBR with a low-
voltage electric field, the joint effects of the electric field force
and electrically released irons alleviated the fouling development.
In the Ti-MBR, no coagulant ions were released from the tita-
nium anode, and besides the effective fouling suppression by the

Fig. 5. Schematic illustration of mechanisms of fouling depression in e-MBR.

230 J. Zhang et al. / Chemical Engineering Journal 273 (2015) 223–230
electric field induced backwash, the properties of the mixed liquor
were affected significantly by the high voltage applied. The MLSS
concentration, mean particle size and SMPs were changed in differ-
ent extents. These parameters would affect the SRF of both the
mixed liquor and the supernatant, and influence the formation
and structure of fouling layers in the Ti-MBR. As shown in Fig. 4,
the SRFs of both the supernatant and the mixed liquor were
increased in the Ti-MBR. The reduction of TMP development in
the Ti-MBR would be due to the electric field force, i.e., the main
mechanism of fouling suppression in the Ti-MBR should be the
electric field induced backwash.
3.4. Implication of e-MBR
In this study, the TMP developments of both e-MBR’s were
depressed compared to the control MBR without an electric field,
and the additional electricity consumption of each e-MBR was
from the application of electric field. The additional specific energy
consumptions were calculated as 0.052 ± 0.002 kWh/m3 in the Fe-
MBR and 0.150 ± 0.002 kWh/m3 in the Ti-MBR. As published, the
total energy consumption of the MBR operation was 0.4–
0.6 kWh/m3 [1]. Thus, in the Fe-MBR, an average of 10% more elec-
tricity resulted in a 30% reduction of TMP. In the Ti-MBR, the reduc-
tion of TMP was not as much as the Fe-MBR, but the additional
energy consumption was on average 30% of the conventional
MBR, and the removal of NH+4-N was inhibited significantly.
Considering its fouling depression with less energy consumption,
and its high efficiency of pollutant removal, the Fe-MBR is a
promising option to be applied in the future.
4. Conclusions
A low-voltage electric field applied into the MBR could effec-
tively alleviate the membrane fouling and enhance the removal
of phosphorus using stainless steel anodes and membrane module
contained cathodes (Fe-MBR). The electric field had two effects:
electric field force and iron ion release. The electric field force on
a negatively charged foulant prevented dense precipitation on
the membrane surface and benefitted the removal of loose fouling
layers. On the other hand, the released iron might react with SMPs
to decrease the TOC and polysaccharide, reducing the foulant and
SRF of the mixed liquor. These joint functions reduced the irrever-
sible fouling and retarded the overall fouling rate. Regarding the
lower additional energy consumption and increased fouling sup-
pression, the Fe-MBR would have great potential for real
application
Acknowledgments
This work was supported by the Science Foundation of the
Ministry of Education of China (No. 20110002130009), the
International Program of MOST (No. 2013DFG92240) and
Program for Changjiang Scholars and Innovative Research Team
in University (No. IRT1152).
Appendix A. Supplementary data
Supplementary data associated with this article can be found, in
the online version, at http://dx.doi.org/10.1016/j.cej.2015.03.044.
References
[1] K. Xiao, Y. Xu, S. Liang, T. Lei, J. Sun, X. Wen, H. Zhang, K. Yu, C. Chen, X. Huang,
Engineering application of membrane bioreactor for wastewater treatment in
China: current state and future prospect, Front. Environ. Sci. Eng. 8 (2014)
805–819.
[2] H. Zhu, W. Li, Bisphenol A removal from synthetic municipal wastewater by
bioreactor coupled with either a forward osmotic membrane or a
microfiltration membrane unit, Front. Environ. Sci. Eng. 7 (2013) 294–300.
[3] S. Liang, K. Xiao, Y. Mo, X. Huang, A novel ZnO nanoparticle blended
polyvinylidene fluoride membrane for anti-irreversible fouling, J. Membr. Sci.
394–395 (2012) 184–192.
[4] J. Wu, F. Chen, X. Huang, W. Geng, X. Wen, Using inorganic coagulants to
control membrane fouling in a submerged membrane bioreactor, Desalination
197 (2006) 124–136.
[5] J. Wu, X. Huang, Use of ozonation to mitigate fouling in a long-term membrane
bioreactor, Bioresour. Technol. 101 (2010) 6019–6027.
[6] J.-P. Chen, C.-Z. Yang, J.-H. Zhou, X.-Y. Wang, Study of the influence of the
electric field on membrane flux of a new type of membrane bioreactor, Chem.
Eng. J. 128 (2007) 177–180.
[7] K. Bani-Melhem, M. Elektorowicz, Development of a novel submerged
membrane electro-bioreactor (SMEBR): performance for fouling reduction,
Environ. Sci. Technol. 44 (2010) 3298–3304.
[8] K. Bani-Melhem, M. Elektorowicz, Performance of the submerged membrane
electro-bioreactor (SMEBR) with iron electrodes for wastewater treatment and
fouling reduction, J. Membr. Sci. 379 (2011) 434–439.
[9] V. Wei, J.A. Oleszkiewicz, M. Elektorowicz, Nutrient removal in an electrically
enhanced membrane bioreactor, Water Sci. Technol. 60 (2009) 3159–3163.
[10] G. Chen, Electrochemical technologies in wastewater treatment, Sep. Purif.
Technol. 38 (2004) 11–41.
[11] K. Akamatsu, Y. Yoshida, T. Suzaki, Y. Sakai, H. Nagamoto, S.-I. Nakao,
Development of a membrane–carbon cloth assembly for submerged
membrane bioreactors to apply an intermittent electric field for fouling
suppression, Sep. Purif. Technol. 88 (2012) 202–207.
[12] L. Liu, J. Liu, B. Gao, F. Yang, Minute electric field reduced membrane fouling
and improved performance of membrane bioreactor, Sep. Purif. Technol. 86
(2012) 106–112.
[13] L. Liu, J. Liu, B. Gao, F. Yang, S. Chellam, Fouling reductions in a membrane
bioreactor using an intermittent electric field and cathodic membrane
modified by vapor phase polymerized pyrrole, J. Membr. Sci. 394–395
(2012) 202–208.
[14] P. Le-Clech, V. Chen, T.A.G. Fane, Fouling in membrane bioreactors used in
wastewater treatment, J. Membr. Sci. 284 (2006) 17–53.
[15] A.A. Wef, Standard Methods for the Examination of Water and Wastewater,
21st ed., Amer. Public. Health Assn, USA, 2005.
[16] J. Wu, X. Huang, Effect of mixed liquor properties on fouling propensity in
membrane bioreactors, J. Membr. Sci. 342 (2009) 88–96.
[17] X.Y. Li, S.F. Yang, Influence of loosely bound extracellular polymeric substances
(EPS) on the flocculation, sedimentation and dewaterability of activated
sludge, Water Res. 41 (2007) 1022–1030.
[18] M. Dubois, K.A. Gilles, J.K. Hamilton, P.A. Rebers, F. Smith, Colorimetric method
for determination of sugars and related substances, Anal. Chem. 28 (1956)
350–356.
[19] B. Frolund, T. Griebe, P.H. Nielsen, Enzymatic-activity in the activated-sludge
floc matrix, Appl. Microbiol. Biotechnol. 43 (1995) 755–761.
[20] Y.-X. Shen, K. Xiao, P. Liang, Y.-W. Ma, X. Huang, Improvement on the modified
Lowry method against interference of divalent cations in soluble protein
measurement, Appl. Microbiol. Biotechnol. 97 (2013) 4167–4178.
[21] K. Xiao, Y. Shen, X. Huang, An analytical model for membrane fouling evolution
associated with gel layer growth during constant pressure stirred dead-end
filtration, J. Membr. Sci. 427 (2013) 139–149.
[22] A. Drews, Membrane fouling in membrane bioreactors – characterisation,
contradictions, cause and cures, J. Membr. Sci. 363 (2010) 1–28.
[23] X.G. Li, H.B. Cao, J.C. Wu, K.T. Yu, Inhibition of the metabolism of nitrifying
bacteria by direct electric current, Biotechnol. Lett. 23 (2001) 705–709.
[24] Y.-X. Shen, K. Xiao, P. Liang, J.-Y. Sun, S.-J. Sai, X. Huang, Characterization of
soluble microbial products in 10 large-scale membrane bioreactors for
municipal wastewater treatment in China, J. Membr. Sci. 415–416 (2012)
336–345.
[25] V. Wei, M. Elektorowicz, J.A. Oleszkiewicz, Influence of electric current on
bacterial viability in wastewater treatment, Water Res. 45 (2011) 5058–5062.
[26] H.M. Huotari, G. Tragardh, I.H. Huisman, Crossflow membrane filtration
enhanced by an external DC electric field: a review, Chem. Eng. Res. Des. 77
(1999) 461–468.
[27] M. Ben Sasson, A. Adin, Fouling mitigation by iron-based electroflocculation in
microfiltration: mechanisms and energy minimization, Water Res. 44 (2010)
3973–3981.
[28] J. Zhang, K. Xiao, P. Liang, T.D. Waite, X. Huang, Electrically released iron for
fouling control in membrane bioreactors: a double-edged sword?,
Desalination 347 (2014) 10–14
[29] B.D. Cho, A.G. Fane, Fouling transients in nominally sub-critical flux operation
of a membrane bioreactor, J. Membr. Sci. 209 (2002) 391–403.
[30] J. Zhang, H.C. Chua, J. Zhou, A.G. Fane, Factors affecting the membrane
performance in submerged membrane bioreactors, J. Membr. Sci. 284 (2006)
54–66.
[31] F. Baldi, D. Marchetto, D. Battistel, S. Daniele, C. Faleri, C. De Castro, R. Lanzetta,
Iron-binding characterization and polysaccharide production by Klebsiella
oxytoca strain isolated from mine acid drainage, J. Appl. Microbiol. 107 (2009)
1241–1250.
[32] I. Arcon, O. Piccolo, S. Paganelli, F. Baldi, XAS analysis of a nanostructured iron
polysaccharide produced anaerobically by a strain of Klebsiella oxytoca,
BioMetals 25 (2012) 875–881.