Biochemical Engineering Journal 133 (2018) 130–139

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Biochemical Engineering Journal

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

Regular article

A new Sponge-GAC-Sponge membrane module for submerged

membrane bioreactor use in hospital wastewater treatment
Qusay F. Alsalhy a,∗ , Faris H. Al-Ani b , Arshed E. Al-Najar b
a
Membrane Technology Research Unit, Chemical Engineering Department, University of Technology, Alsinaa Street 52, Baghdad, Iraq
b
Building and Construction Engineering Department, University of Technology, Alsinaa Street 52, Baghdad, Iraq

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

Article history: A new Sponge-GAC-Sponge membrane module design for use in a membrane bioreactor (SGSMBR)
Received 9 January 2018 is presented in this study. This work highlights an alternative MBR design in which a composite
Accepted 11 February 2018 Sponge-Granular Activated Carbon-Sponge (SGS) layer is covered around the membrane module. The
Available online 12 February 2018
performance and membrane fouling of both the SGSMBR and a University of Cape Town with membrane
(UCT-MBR) system are investigated for use in hospital wastewater treatment. It has been found that
Keywords:
decreasing the hydraulic retention time (HRT) from 8 to 4 h resulted in higher COD, NH3 , and P removal
Membrane bioreactor
efficiency in the SGSMBR process when compared with the UCT-MBR process. Membrane fouling is con-
Sponge layer
PVC ultrafiltration
trolled in the SGSMBR by decreasing the cake layer thickness on the membrane surface by about 96%. The
Cake layer flux recovery efficiency (FRE%) of the membranes was highly improved in the new SGSMBR design. The
Membrane fouling COD, NH3 , and P removal efficiency was improved significantly from 73.6, 84.9, and 58% by using UCT-
MBR to 85, 96, and 71%, respectively by using UCT-SGSMBR and SGSMBR. Finally, the SGSMBR showed
biomass retention superior to that measured in the UCT-MBR. This work reveals, for the first time, that a
composite layer covering the membrane module is a viable alternative to anoxic and anaerobic conditions
in MBR systems.
© 2018 Elsevier B.V. All rights reserved.

1. Introduction However, fouling, and bio-fouling in particular, acutely affects

In recent decades, membrane bioreactor (MBR) systems have
emerged as a suitable alternative to traditional biological recla-
mation processes for carbon source as well as nutrient removal
[1]. MBRs have several advantages, including high removal effi-
ciency [1], low space requirements, perfect total solids removal,
low sludge generation, and perfect retention of biomass inside the
system [2,3].
Abbreviations: SGSMBR, sponge – granular activated carbon – sponge – mem-
brane bioreactor; SGS, sponge – granular activated carbon – sponge; UCT-MBR,
University of Cape Town with membrane; HRT, hydraulic retention time; SRT, solids
retention time; COD, chemical oxygen demand; FRE, flux recovery efficiency; GAC,
granular activated carbon; MBR, membrane bioreactor; GBF, green bioflocculant;
WWTP, wastewater treatment plant; CIP, chemical cleaning-in-place; PAC, powder
activated carbon; EPSs, extracellular polymeric substances; SMBR, sponge mem-
brane bioreactor; PVC, polyvinyl chloride; DMAc, dimethylacetamide; PWP, pure
water permeability; AS, activated sludge; MLSS, mixed liquor suspended solid; BAG,
biomass attached growth; ZnO, zinc oxide; DO, sissolved oxygen.
∗ Corresponding author.
E-mail address: 80006@uotechnology.edu.iq (Q.F. Alsalhy).
MBR processes. Generally, bio-fouling occurs via the accumulation
of biomass at a membrane surface due to inorganic precipitation
and adhesion of bacterial cells to the surface of the membrane [4,5].
One of the most serious operational problems encountered in MBR
systems, bio-fouling causes rapid declines in the permeate flux,
reduced membrane productivity, excess membrane substitution,
and increased operational costs.
Various methods have been used in MBRs to decrease fouling
of the membrane. Ngo and Guo [6] reported that the distributed
injection of air through submerged MBR (SMBR) processes, along
with the addition of low-dosage green bioflocculant (GBF), reduced
layer fouling to nearly zero after 70 d of operation; this method
also reduced backwash recurrence. Wei et al., [7] was explored a
chemical cleaning-in-place (CIP) method for treatment of domestic
wastewater in a long-term, pilot-scale operation using MBRs. The
use of a biomass support medium such as powder activated car-
bon (PAC), plastic media, and sponges in MBRs is a powerful and
promising strategy for membrane fouling control [8,9]. Combina-
tions of a MBR and PAC, in which PAC is used as a pre-treatment
before membrane technology, have proven promising in wastew-
ater pre-treatment.

https://doi.org/10.1016/j.bej.2018.02.007
1369-703X/© 2018 Elsevier B.V. All rights reserved.
 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139
Nomenclature
Symbols
V Volume (m3 )
t Time (h)
A Area (m2 )
P Transmembrane pressure (bar)
R Removal efficiency (%)
Cp Pollutant concentrations of the influent (mg/L)
Cf Pollutant concentrations of the effluent (mg/L)
J Flux ((l/m2 h)
M Mass of the permeated water (l)
A Effective membrane area (m2 )
Actually, higher concentrations of PAC in the MBR resulted in
better adsorption, deterioration, and biodegradation and reduced
Mixed Liquor Suspended Solid (MLSS) fouling components such
as Extracellular Polymeric Substances (EPSs) and fine colloids
[10]. Sponges are considered to be ideal attached-growth mate-
rial as they can be used as a transportation medium for active
biomass, decrease cake layer accumulation on the membrane sur-
face and retain biomass by encouraging a hybrid growth system
(that combines suspended and attached growth) [10,11]. Sponges
have performed well in biological treatments because of several
advantages, for example; high interior porosity and specific sur-
face area, high stability to hydrolyses, light weight and economy
[10,12].
The impact on nitrogen removal of using a sponge cube
as a biomass supported medium was studied by Deguchi and
Kashiwaya [13]. They found that the rates of nitrification and den-
itrification in the sponge system were higher than those measured
in a suspended growth reactor by 1.5 and 1.6 times, respectively.
Guo et al., [14] studied the impacts on fouling and permeate flux
of the membrane of suspending a cubic sponge in the tank of the
SMBR. They reported that the suspended-sponge membrane pro-
cess, in which the sponge filled 10% of the tank volume, decreased
membrane fouling and enhanced the sustainable flux by 100% over
that of the SMBR alone. Nguyen et al., [3] demonstrated that the
suspended sponge membrane bioreactor (SSMBR) succeeded in
decreasing membrane fouling and had high organic carbon and
nutrient removal efficiencies.
Moreover, the influence of sponge size and type on the perfor-
mance of a conventional biological system was reported by Nguyen
et al., [15]. They used sponges of types S28-30/45R, S28-30/60R,
S28-30/80R and S28-30/90R with dimensions of 1 cm3 , 2 cm3 and
3 cm3 . The results indicated similar removal efficiencies for nutri-
ents and organic substances among the various types of sponge.
The studies mentioned above explored the effects of introduc-
ing cubic sponges and granular activated carbon (GAC) to the MBR
tank, finding that these additions improved treatment performance
and decreased membrane fouling. Indeed, the direct addition of the
cubic sponge to the bioreactor causes mixing with the activated
sludge, making it impossible to separate the sponges and the sludge
at the end of the process. Also while the addition of GAC causes a
significant reduction in membrane fouling, it is not possible to reuse
the GAC again. We therefore focus on, and solve, these problems in
this study.
This study presents a new Sponge-GAC-Sponge membrane
module in a membrane bioreactor (SGSMBR) design. This work
highlights an alternative MBR design in which a composite layer,
composed of three sub-layers made of Sponge-Granular Activated
Carbon-Sponge (SGS), is covered around the membrane module
instead of distributing the cubic sponges and granular activated
carbon throughout the MBR tank. In this design, the composite
131
layer around the membrane module functions as an alternative to
the aerobic, anoxic and anaerobic conditions in typical MBR sys-
tems; specifically, the first sponge sub-layer (at the outer surface
of the composite layer) works as an alternative to aerobic condi-
tioning, the second sub-layer (i.e., the internal porous surfaces of
the sponge and granular activated carbon) works as an alterna-
tive to anoxic conditioning, and the third sponge sub-layer works
as an alternative to anaerobic conditioning, as the previous two
sub-layers prevent dissolved oxygen transport to this final sub-
layer. Other benefits of this MBR design include low cost due to the
possibility of reactivating sub-layers through periodic cleaning as
well as reduced membrane fouling, enhanced permeation flux and
improved phosphorus and nitrogen removal. Moreover, this new
method facilitates long-term maintenance in SGSMBR processes.
The objectives of this study are investigating the effects of a
new sponge-granular activated carbon composite layer covered the
membrane on the performance of a SGSMBR for actual hospital
wastewater treatment, examining the effects of the SGS composite
layer on biomass growth on sponge surfaces and interior sub-layers
as well as on the cake layer thickness on the membrane surface
are evaluated, proving that the SGS composite layer covered the
membrane module works as an alternative to the anoxic and anaer-
obic conditions in typical MBR systems; and studying effects of
hydraulic retention time (HRT) on the COD, NH3 , and P removal effi-
ciency in the SGSMBR process when compared with the UCT-MBR
process. In addition, a comparison was conducted in an effort to
evaluate the performance of UCT-MBR, UCT-SGSMBR and SGSMBR
systems.
2. Material and methods
2.1. Materials
PVC resins of 65 kg/mol were used as membrane materials and
were obtained from the Georgia Gulf Company (Georgia, USA). N,
N-dimethylacetamide (DMAc) solvents were supplied by Sigma-
Aldrich. ZnO nanoparticles (99%; 10–30 nm in diameter; Product
No. 8411DL) were purchased from SSNano, USA.
2.2. Membrane preparation
The PVC polymer material was dried at 60 ◦ C in an oven for 4 h to
remove moisture. The casting solution was prepared through the
addition of dried 10 wt.% PVC to 90 wt.% N,N-dimethylacetamide
(DMAc) solvent. The PVC was mixed with the DMAc using a mag-
netic stirrer for 2 d at 200 rpm and 40 ◦ C until homogeneity was
achieved, after which the inorganic ZnO nanoparticles were added.
Then, the final casting solution with ZnO nanoparticles was placed
in an Ultrasonic water bath for 15 min to prevent ZnO nanoparticle
aggregation in the final casting solution.
The polymer solutions were cast with 200 ␮m thicknesses uti-
lizing a motorized film applicator (CX4 mtvmesstechnik, Germany)
under atmospheric conditions. The prepared membranes were sub-
merged in a non-solvent coagulation bath (i.e., deionized water) at
room temperature for deposition. The nascent membrane was kept
in tap water for 48 h to remove the remaining DMAc. Finally, the
membrane was moved and kept in a 30 wt% glycerol solution for
48 h to protect the membrane structure from collapse and crack-
ing. Three identical membrane sheets were selected for membrane
characterization and used in ultrafiltration UF tests to procure mean
flux and pollutant removal values.
132 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139
2.3. Characterization of the membrane surface
2.3.1. Scanning electron microscopy
SEM is a common technique used to analyse the structure
of a prepared membrane. SEM images were made with a TES-
CAN VEGA3 SB instrument (EO Elektronen-Optik-Service GmbH,
Germany) with an accelerating voltage of 30 KV. Cross-sections of
the flat sheet membranes were obtained via freeze fracturing in
liquid nitrogen to obtain a clean, brittle fracture.
2.3.2. Atomic force microscope
The flat-sheet membrane was subjected to broad surface exami-
nation using an AFM made by Angstrom Advanced Inc. (USA; model
AA3000) in contact mode with a reusable silicon tip. The observa-
tions obtained include appraisal of the topography (the rise and fall
of the sample surface), the lateral force, and the deviation. Measur-
able pore estimate dissemination was set up using the IMAGER 4.31
program for the external surfaces of each flat-sheet membrane.
2.4. Permeation flux and the removal of pollutants
The water flux and pollutants removal studies for the mem-
branes were conducted using cross-flow filtration experiments. All
experiments were performed in cross flow mode with a membrane
cell under a −0.4 bar vacuum using a feed solution temperature of
25 ◦ C. The effective membrane area was 18 cm2 . The volume of the
solution was 5 L. Permeate was collected in a graduated cylinder
until it reached steady state. Pure water permeability (PWP) was
calculated as follows:
V were fed hospital wastewater from a storage tank via a feed suc-
PWP =
t.A.P
where PWP is the PWP of the membrane (l/(m2 h bar)), V is the
volume collected (L), t is permeate collection time (h), P is the
transmembrane pressure, and A is the membrane surface area (m2 ).
The removal R (%) of the dissolved pollutant was calculated as
follows:
 Cp
 membrane modules were installed in the MBR. Air was injected
R(%) = 1− × 100
Cf
where Cf and Cp are the pollutant concentrations of the influent
and effluent, respectively.
2.5. Membrane fouling analysis
Antifouling and permeation experiments of PVC/ZnO flat-sheet
membrane were carried out under constant vacuum of −0.4 bar for
pure water and AS with an MLSS of 10000 mg/L to prevent com-
paction effects in the membrane. The membrane pure water flux
was measured by applying a −0.4 bar vacuum for 30 min before the
main flux test. The permeation flux was measured for 90 min and
calculated as follows:
M
J=
A.t
where J, M, t and A are the permeation flux, mass of the permeated
water, permeation time and effective membrane area, respectively.
Then, sludge filtration was performed in the UCT-MBR process
shown in Fig. 1 for 90 min. Next, the flat sheet membranes were
ejected from the MBR and cleaned gently with distilled water, after
which the pure water flux was measured to check the flux recovery
efficiency (FRE) of the flat sheet membranes, which was calculated
as follows:
 
Jwater,2
FRE (%) × 100
Jwater,1
where Jwater,1 and Jwater,2 are the flux before and after the MBR test,
respectively.
2.6. Sponges
In the SGSMBR system, two kinds of polyester-urethane sponges
(PUSs) were used: coarse pore structure (S 28–30/45R) (density
of 28–30 kg/m3 with 45 cells per 25 mm) and fine pore structure
(S 16–18/80R) (density of 16–18 kg/m3 with 80 cells per 25 mm).
The dimensions of both the coarse and fine pore structure sponge
sheets were 9.5 × 15.5 × 1.5 cm3 . The two types of sponge were pur-
chased from Al-Hillal Company for sponge industry, Baghdad, Iraq,
whereas the GAC were purchased from ROMIL PURE CHEMISTRY,
Cambridge GB-CB259QT.
2.7. Sponge-GAC-Sponge membrane bioreactor (SGSMBR)
configuration
The PVC/ZnO flat sheet membrane module had an average pore
size of 211 nm, as evaluated by AFM, and a surface area of 18 cm2 .
The membrane cell was covered in three sub layers above the
PVC/ZnO flat sheet membrane cell as shown in Fig. 2. The top layer
is formed from coarse-pore-structure sponge, the middle layer con-
tains GAC, and the bottom layer is comprised of fine-pore-structure
sponge, as shown in Fig. 2.
2.8. Experimental setup
The experiment was conducted using three pilot plants, which
(1)
tion pump. This actual wastewater was collected downstream of
a wastewater treatment plant (WWTP) located in Hilla hospital
(Iraq).
The pilot plant composed of a UCT-MBR as shown in Fig. 1a;
the UCT-MBR composed of three tanks: an anaerobic tank (8.0 L),
an anoxic tank (16 L), and the MBR (32 L). The PVC/ZnO flat-sheet
(2) at the base of the aerobic tank to supply oxygen for microorgan-
isms and reduce fouling on the membrane. The anaerobic tank and
the anoxic tank each contained one stirrer. Mixed liquors from the
MBR tank were returned to the anoxic tank (Recirculation 1) and
then, from anoxic tank to the anaerobic tank (Recirculation 2) by
two pumps. Hospital wastewater was pumped into the anaerobic
tank from the storage tank. COD was consumed partially and phos-
phorus was released in the chamber of anaerobic process. Then,
the effluent moved to the anoxic tank and the MBR. Organic matter
oxidation, nitrification and phosphorus accumulation occurred in
the aerobic zones. Recirculation 1 consisted of NO3 recirculation
from the membrane tank to the bioreactor anoxic chamber, which
permitted nitrogen removal and reduced the impact of nitrate in
wastewater come in the anaerobic zone. Recirculation 2 is refers
to the returned wastewater to anaerobic tank from anoxic cham-
(3) ber in order to increase the organic matter utilization and provided
the optimal conditions for fermentation of organic material and
phosphorus uptake in the anaerobic tank.
The UCT-SGSMBR is shown in Fig. 1a; the UCT-SGSMBR is the
same as the UCT-MBR in construction and operation except for the
addition of the multilayer sponge covering the membrane cell. A
schematic of the SGSMBR is presented in Fig. 1b; the effective vol-
ume of the bioreactor was 32 L. Actual wastewater was pumped
into the reactor using a feeding pump to control the feed rate while
the effluent flow rate was controlled by a suction pump. Level sen-
sor was used to control the wastewater volume in the reactor. A
(4) pressure gauge was used to measure the TMP and air was injected
at the base of the aerobic tank to supply oxygen for microorgan-
 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139 133

Fig. 1. Schematic diagram of: A) the lab-scale of UCT-MBR and UCT-SGSMBR B) SGSMBR system.

Fig. 2. SGSMBR membrane module.

134 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139

Table 1
Operating conditions and working concentration of MLSS in the steady state.

Parameter Run 1 Run 2 Run 3 2.10. Assessment of water quality

UCT-MBR UCT-SSMBR SSMBR

ZnO (wt.%) 0.1 0.1 0.1 Influents and membrane effluents were gathered from the UCT-
PVC (wt.%) 10 10 10
MBR for estimation of conventional parameters. COD, MLSS, NH3 ,
Volume (L) anaerobic 8 8 0
anoxic 16 16 0
and P were determined in accordance with common Standard
aerobic 32 32 32 Methods (APHA, 2005).
HRT (h) anaerobic 2 2 0
anoxic 4 4 0
aerobic 8 8 4
3. Results and discussion
SRT (d) 25 25 25
MLSS (g/L) 10 10 10 3.1. Membrane properties
Vacuum (bar) 0.4 0.4 0.4
Operation time (d) 21 21 21
Fig. 3 shows three AFM images of the top surface of the PVC
membranes and SEM images of the cross-sectional structure of the
membranes prepared with 0.1 g of ZnO nanoparticles in casting
isms. The SGSMBR was filled with sludge from the local Wastewater
solution. In these AFM images, the dark regions are valleys (i.e.,
Treatment Plant and acclimatized to actual wastewater.
pores) and the bright regions are high points or nodules. It can be
seen that the nodular aggregates have merged together to form a
2.9. Process operating conditions number of string-like structures with ZnO nanoparticles.
The AFM technique reveals that the average roughness and pore
The bioreactor was initially filled with seed sludge obtained diameter of the PVC/ZnO flat sheet membrane are 21.5 (±2.2) nm
from Al-Rustumia Treatment Plant, Baghdad. The stabilization and 211.32 (±5.64) nm, respectively. Regarding the structure of the
period for each MBR configuration prior to the 21 days of operation cross-section of the membrane, it can be noticed from Fig. 3B that
was 45 days. The initial MLSS was 1.5 (±0.09) g/L, and during the the cross-sectional structure of the membrane is composed of two
stabilization period, MLSS become 8.8 (±1.1) g/L. In the UCT-MBR micro-void structure.
the concentration of the dissolved oxygen (DO) was kept within
1–4 mg/L in the aerobic zone, while DO in the anoxic and anaero-
3.2. COD removal
bic zones was limited to <0.2 mg/L and <0.1 mg/L, respectively. To
maintain a constant temperature of 25 ± 2 ◦ C in the system, a tem-
Fig. 4 presents the changes in influent and effluent COD and
perature controller was used. The rates of Recirculations 1 and 2
the COD removal efficiency as function of time for UCT-MBR, UCT-
were respectively, 300% and 100% from the influent. An interrupted
SGS-MBR, and SGSMBR experiments. For UCT-MBR experiment at
filtration method, which consisted of 10 min of suction after 1 min
HRT = 8 h, the influent COD concentration fluctuates extensively,
of repose, was adopted in this effort. The MBR was operated under
ranging between 0.99 (±0.05) and 10.3 (±0.08) mg/L. However,
a constant vacuum (−0.4 bar). The hydraulic retention time (HRT)
the removal efficiency is approximately 73.6% (±0.8) in the UCT-
was maintained at about 2 h for anaerobic processing, 4 h for anoxic
MBR as shown in Fig. 4a. The influent COD during the UCT-SGSMBR
processing and 8 h for aerobic processing, while the solids reten-
experiment at HRT = 8 h varies between 0.825 (±0.06) and 0.88
tion time (SRT) was fixed at 25 d per the optimum experimental
(±0.11) mg/L as shown in Fig. 4b. It can be observed that the
conditions found in Brown et al., and Metcalf and Eddy [16,17]. The
COD removal efficiency measures 85.1% (±2.6). Regarding SGSMBR
operating conditions and working concentrations of the MLSS in
experiment, the influent COD concentration fluctuates extensively,
this study are shown in Table 1.
ranging between 700 and 860 mg/L in Fig. 4c. However, the removal
Moreover, in Al-Hilla hospital, south of Baghdad, Iraq, where
efficiency is approximately 85% in the SGSMBR when the HRT is
surgical operations are carried out within 7 days each month;
decreased from 8 to 4 h (i.e., HRT decreased by 50%).
hence, throughout this period of time the characteristics of the
The lack of a significant reduction in COD removal with decreas-
actual wastewater that collected downstream by wastewater treat-
ing HRT may be explained by the use of the sponge layer as a porous
ment plant (WWTP) is significantly changed due to the blood
biomass support increasing the possibility of contact between
disposal procedures in the sanitary network, which may lead to
microorganisms and the organic substrate. The current study shows
an highly increase in the concentration of organic compounds and
that HRT has a negligible impact on COD removal. The SGSMBR sys-
nutrients. For that reason, it is prefer to conduct the wastewater
tem has succeeded in removing COD with a decrease in the HRT
treatment experiments only 21 days each month.
from 8 to 4 h. This suggests that the new SGSMBR can be oper-
Regarding the measurement of the MLSS in each layer, the
ated with a short HRT because of much higher concentrations of
sponge was squeezed and rinsed with distilled water in order to
microorganisms developed in the solid than in the suspension;
remove all of biomass out of the sponge, and the following equation
therefore the rate of degrading of the substrate is higher.
was used to calculate the amount of MLSS:

MLSS = (dry weight of residue and filter
− dry weight of filter alone, in gm)/mL of sample
While the amount of MLSS remaining in the sponge was calcu-
lated as follows:
MLSS = (dry weight of residue and filter (sponge)
− dry weight of filter (sponge) alone, in gm)/mL of sample
3.3. Nitrification and denitrification
(5)
Fig. 5 shows NH3 removal in the UCT-MBR, UCT-SGS-MBR, and
SGSMBR systems. In UCT-MBR experimental configuration (Fig. 5a),
the HRT is 8 h, the average influent NH3 concentration is 166 (±4.6)
mg/L and the average removal efficiency is 84.9% (±3.1), with efflu-
ent concentrations of 24.9 (±1.7) mg/L. These results indicate good
nitrification in the system. In the UCT-SGSMBR experimental con-
figuration, the HRT is 8 h, the average influent NH3 concentration
is 156.4 (±3.1) mg/L, and the average removal efficiency is 96.7%
(6) (±2.1), with effluent concentrations of 5 (±0.5) mg/L as shown
 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139 135

Fig. 3. AFM and SEM images of the PVC/ZnO flat sheet membrane.

in Fig. 5b. These values indicate that nitrification and denitrifica-
tion are entirely complete in this system. This increment may be
explained by additional denitrification in the sponge layer. The
surface of the coarse sponge, which consists of large pore sizes,
can host nitrifying and denitrifying bacterial growth, where the
top surface of the sponge represents an aerobic microenvironment
and the inner surface represents an anoxic microenvironment; this
results in more aerobic bacteria on the top surface and more anoxic
bacteria on the inner surface. In the SGSMBR experimental con-
figuration, the HRT is decreased to 4 h, the average influent NH3
concentration is 158 (±2.4) mg/L and the average removal effi-
ciency is 96.6% (±0.8), with effluent concentrations of 5.2 (±0.7)
mg/L as shown in Fig. 5c. These values indicate that nitrification
and denitrification are entirely complete in this system, which has
a HRT of 4 h and does not use either anaerobic or anoxic tanks.
136 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139
Fig. 4. COD concentrations and removal efficiency for a: UCT-MBR, b: UCT-SGS-
MBR, and c: SGSMBR experiments.
Fig. 5. NH3 concentrations and removal efficiency for a: UCT-MBR, b: UCT-SGS-MBR,
and c: SGSMBR experiments.
SGSMBR is the best configuration for the treatment of nutrients
due to the sponge layer, which is a perfect connected development
medium because it can act as a biomass support medium. Moreover,
the enhancement of the nutrient removal efficiency is attributed to
the trapped of the large amount of biomass in the sponges, much
higher concentrations of microorganisms developed in the solid
than in the suspension, therefore the rate of degrading the substrate
is higher and accordingly increases the nitrification and denitrifi-
cation. Deguchi and Kashiwaya [13] found that the nitrification and
denitrification rates in the sponge system were 1.5 and 1.6 times
higher, respectively, than those measured in a suspended growth
reactor.
Cho et al., [18] found that the nutrient removal efficiency was
higher under short HRTs than under long HRTs; increasing the HRT
by 30% resulted in a 10% decrease in the nutrient removal effi-
ciency. However, the short HRT and high flux resulted in increased
membrane fouling. It is clear from the SGSMBR results that deni-
trification is completed even with a short HRT and that the system
is not affected by membrane fouling.
SGSMBR located in the aerobic tank is the best nutrient treat-
ment configuration because nitrification and denitrification occur
in the same (aerobic) tank, eliminating the need for anaerobic
and anoxic tanks. Neither membrane fouling nor treatment per-
formance is affected by operation under low HRT and high SRT.
Higher NH3 removal in the SGSMBR may be caused by the pro-
motion of biomass-oxidizing bacteria on the sponge layer, which
provides anoxic conditions in the inner pores and on the bottom
layer of the sponge.
NO3 removal in the UCT-MBR, UCT-SGSMBR and SGSMBR exper-
iments is summarized in Fig. 6. NO3 concentrations are 45 (±1.6)
mg/L in the influent and 30.2 (±2.1) mg/L in the effluent for the
UCT-MBR configuration; 45 (±1.9) and 0 mg/L in the influent and
effluent, respectively, for the UCT-SGSMBR configuration (when the
HRT = 8 h and the SRT = 25 d); and 45.8 (±2.3) and 0 mg/L in the
influent and effluent, respectively, for the SGSMBR configuration
Fig. 6. NO3 influent and effluent concentration for UCT-MBR, UCT-SGSMBR, and
SGSMBR experiments.
Fig. 7. P concentrations and removal efficiency for a: UCT-MBR, b: UCT-SGSMBR,
and c: SGSMBR experiments.
(when the HRT = 4 h). These results indicate complete denitrifica-
tion in the SGSMBR systems.
3.4. Phosphorus removal
Fig. 7 shows variations in influent and effluent P and P removal
efficiency as a function of time in the UCT-MBR, UCT-SGS-MBR,
and SGSMBR systems. The performance of the UCT-MBR system
has been investigated for 21 d using a submerged PVC/ZnO flat
sheet MBR. The influent P concentration fluctuates extensively
from 16 to 18 mg/L. The phosphorus removal efficiency is stable
at approximately 58% as shown in Fig. 7a. A simple bio-P removal
process must include at least two stages, including a non-aerated
stage and an aerated stage. In the first stage, influent wastewater
and returned sludge are combined under non-aerated conditions.
Phosphate release from the biomass and soluble chemical oxygen
demand (COD) removal are observed under these anaerobic condi-
tions in the absence of both oxygen and nitrate. In the subsequent
aerated stage, phosphate removal, COD removal and nitrification
occur. Phosphorus-rich sludge from this aerobic reactor is usually
discarded. Many processes also include an intermediate denitrifica-
tion stage, often referred to as an “anoxic” stage, in which nitrified
mixed liquor is recycled from the aerated reactor. Barnard [19,20]
showed that phosphate release under non-aerated conditions is a
prerequisite to subsequent aerobic phosphate uptake.
In the UCT-SGSMBR experimental configuration (Fig. 7b), the
HRT is 8 h, the average influent P concentration is 17.5 (±0.9) mg/L
and the average removal efficiency is 71.2% (±0.9), with effluent
concentrations of 5.04 mg/L and the performance of this system
has been investigated for 21 d. In the SGSMBR experimental con-
figuration (Fig. 7c), the performance has been investigated for 21 d,
the HRT is 4 h, the average influent P concentration is 17.4 (±1.2)
mg/L and the average removal efficiency is 71.1% (±1.2), with efflu-
ent concentrations of 5 (±0.65) mg/L. The results also indicate that
 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139 137

Fig. 9. Flux recovery efficiency (FRE) of the UCT-MBR and SGSMBR.

Fig. 8. Flux of pure water and filtration of activated sludge in MBR versus time for
the UCT-MBR and SGSMBR.

P removal decreases after 5–12 d. The results show that the sponge
layer is an ideal biomass support medium for the SGSMBR system.
Sponge with fine pore structure has an effect on the removal of P
due to the small size of the floc, where the small size of the organic
matter particles affects the rate of the hydrolysis. This is because
the small particles size has a larger surface area and thus degrades
rapidly with reduction of the stabilization time compared to large
particles
The P removal (effluent P < 5.0 mg/L) also indicates that
increased biological phosphorus removal, as well as excess phos-
phorus uptake, can be achieved by the accumulation of phosphate
organisms on the sponge layer. Furthermore, microorganisms
attached to the sponge and in the MLSS remove a portion of the
phosphorus biologically, as P is an essential nutrient for biomass Fig. 10. Bio-layer of the UCT-MBR and SGSMBR.
growth [21]. According to the COD, NH3 , and P removal data, the
SGSMBR system succeeds due to the composite layer around the
membrane module, which provides an alternative to anoxic and
anaerobic processing in the MBR system. SGSMBR is an alterna-
tive technique for treatment of wastewater to traditional UCT-MBR
technique. It shows many advantages such as capable of high nitro-
gen and phosphorus removal, simple operation, low cost, small area
required, membrane fouling controlled, and alternative to anoxic
and anaerobic condition.

3.5. Membrane antifouling performance and long-term operation

Membranes that are used for MBR processes shown in Fig. 1

should be able to recover, in terms of water flux, after being in
contact with sludge. Therefore, it is necessary to compare the mem-
brane water flux before and after activated sludge filtration. After
the activated sludge ultrafiltration test, the membranes were gen-
tly cleaned and the pure water fluxes were measured again; the
results are shown in Fig. 8. Flux through the membranes reaches a
nearly steady value over time, and the water flux is much higher
than the sludge flux. The membrane fouling resistance is usually
evaluated using the FRE value. Higher FRE values indicate better
membrane antifouling ability during the ultrafiltration process. As
can be seen in Fig. 9, the FRE value is 60% (±2) for the UCT-MBR and
95.3% (±3.5) for the SGSMBR.
In Fig. 10 the decrease in the cake layer with the addition of a
sponge layer is clear; because the MLSS is not attached directly to
the membrane, and the multilayer sponge prevented the activated
sludge from moving to the MBR. The cake layer is 36.87 ␮m thick
in the UCT-MBR (difference between bio-layer thickness after and
before the process) as shown in Fig. 10, where the addition of the
multilayer sponge is decreases the cake to 1.58 ␮m in the SGSMBR.
In fact, SGS module acts like the “real” membrane, the PVC/ZnO
membrane having, merely, the role of finishing the treatment and
preventing some microorganisms to leave with the treated water.
The SGS module can solve the issue of cake formation so prevalent
Fig. 11. Permeate flux versus time for long-term experiment for UCT-MBR and
SGSMBR.
in traditional MBRs. Yang et al., [22] reported that a Sponge-MBR
system was proficient at controlling membrane fouling, and espe-
cially the cake layer on the membrane. The result was an 86%
reduction in cake resistance and a 20% flux increase compared to
the MBR alone.
Regarding the long-term operation, permeate flux against
elapsed time for the long-term (21 day) experiment for UCT-MBR
and SGSMBR is presented in Fig. 11. It can be seen that the permeate
flux in the UCT-MBR configuration has started with 33.4 (±0.88)
L/m2 .h and after long-term operation of 21 d, the permeate flux
decline to 24 L/m2 .h, whereas in the SGSMBR configuration the per-
meate flux has started with 63.8 L/m2 .h and after 21 d of long-term
operation the permeate flux slightly decreased to 63.3 L/m2 .h. In
fact, the sponge/GAC acts as a pre-filter and prevents accumula-
tion of too much biomass on the membrane during the long-term
operation.
It is worth to mention here for the first time that the concept
of the sponge/GAC pre-filtration is new and very interesting. It is
clear that this pre-filtration will long-term in fact be beneficial and
138 Q.F. Alsalhy et al. / Biochemical Engineering Journal 133 (2018) 130–139
Fig. 12. MLSS variation of the activated sludge of the experiments.
this pre-filter will accumulate too much biomass and protecting
the polymeric membrane.
3.6. MLSS in activated sludge
MLSS levels in the activated sludge in the UCT-MBR and biomass
attached growth (BAG) in the SGSMBR experiments are presented
in Fig. 12. Every day, MLSS was tested in order to monitor the phys-
ical properties of the activated sludge. The MLSS is 10 g/L in the
UCT-MBR. In the SGSMBR, the BAG can be divided into two types of
microorganisms: the BAG in the upper sponge layer aerobic zone
(which has a coarse pore structure), and that in the lower-layer
anaerobic zone (which has a fine pore structure). The activated
sludge content was measured at the beginning of the experi-
ment. The MLSS development rates are 26.7(±0.03) (g biomass/g
sponge) and 1.7 (±0.01) (g biomass/g sponge) in the upper and
lower layers, respectively. The results indicate that the BAG in the
SGSMBR was higher than that in the UCT-MBR. The coarse layer
has more attached biomass than does the fine layer, which leads to
increased denitrification due to the anoxic environment provided
and increases the flux to the second layer. The fine-pore layer has
better P removal because the previous two sub-layers prevent the
transport of dissolved oxygen (DO) to the final layer, creating an
anaerobic environment. Additionally, the small pore size prevents
large floc and microorganisms from attaching and/or adhering to
the membrane surface, reducing membrane fouling.
In general, a high MLSS concentration is not favorable in the
bioreactor because it increases the sludge viscosity as well as it
does membrane fouling. Meng et al., [23] found that high MLSS
concentrations were the main cause of high viscosity due to the
presence of EPS. Meng et al., [24] was found similar observations,
which suggested that sludge viscosity was affected by the MLSS
concentration, EPS and filamentous bacteria. In this study, high
MLSS concentrations do not affect the viscosity or the fouling rate.
In general, the SGSMBR shows better biomass retention than does
the UCT-MBR because of biomass entrapment in the sponge layer.
3.7. Identification of bacteria
Three samples were taken from the sponge. Sample No. 1 was
taken from the top sponge layer (1 st coarse sponge layer from the
surface facing the bioreactor) and Sample No. 2 was taken from
the bottom sponge layer (1 st coarse sponge layer from the sur-
face facing the GAC layer) in order to identify the types of bacteria
present and to improve the aerobic and anoxic environments in
the same layers. Sample No. 3 was taken from the second sponge
layer (i.e., the surface facing the membrane) to improve the anaer-
obic environment. The samples were cultured on different media,
including MacConkey’s agar, Blood agar, Eosin methylene blue agar,
and Nutrient agar, under aerobic, anoxic, and anaerobic conditions.
Table 2
The types of bacteria isolated from the sponges.
Condition Name of bacteria
Aerobic Escherichia coli
Enterobacter sp.
Bacillus subtilis
Klebsiella pneumoniae
Proteus mirabilis
Anoxic Streptococcus intermedius
Anaerobic Actinomyces sp.
The bacteria were isolated and investigated using different bio-
chemical tests and the Gram stain procedure [25]. Table 2 shows the
types of bacteria isolated from the two types of sponges. The types
of bacteria isolated from the two types of sponges confirmed our
hypothesis that the composite layer covered the membrane module
working as an alternative to aerobic, anoxic and anaerobic pro-
cessing in the MBR system; for example, the first sponge sub-layer
at the outer surface working as an alternative to aerobic process-
ing, the second sub-layer (i.e., the internal porous surfaces of the
sponge and granular activated carbon) functions as an alternative
to anoxic processing, and the third sub-layer of sponge functions
as an alternative to anaerobic processing.
4. Conclusions
A new membrane module design involving a SGSMBR is consid-
ered in this work. This is the first work to investigate the effects of
using a sponge-granular activated carbon composite layer covered
around the membrane on the performance and operating parame-
ters of a SGSMBR for actual hospital wastewater treatment.
The essential conclusions of this work are:
• Using the new SGS composite layer module design, the COD, NH3
and P removal efficiencies are improved from 73.6%, 84.9% and
58%, with an 8-h HRT in the UCT-MBR to 85%, 96.6% and 71.1%,
respectively, with a shorter HRT of 4 h. These removal efficien-
cies increase because large amount of biomass are trapped in the
sponges, which increases nitrification and denitrification.
• Membrane fouling is controlled by reducing the cake layer thick-
ness on the membrane surface in the SGSMBR by approximately
96%.
• The membrane flux recovery efficiency (FRE%) is substantially
improved in the new SGSMBR design because microorganisms
are not directly attached to the membrane; the multilayer sponge
prevents the transport of the activated sludge to the MBR.
• The composite layer covered the membrane module works as
an alternative to anoxic and anaerobic conditioning in the MBR
system.
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