Inuence of sludge retention time on membrane fouling

and bioactivities in membrane

bioreactor system
Sung-Soo Han
a,b
, Tae-Hyun Bae
a
, Gyung-Gug Jang
a
, Tae-Moon Tak
a,
*
a
School of Biological Resources and Materials Engineering, Seoul National University, San 56-1,
Shinlim-dong, Kwanak-ku, Seoul 151-744, South Korea
b
School of Civil and Environmental Engineering, Georgia Institute of Technology,
Atlanta, Georgia, GA 30332, USA
Received 7 June 2004; received in revised form 13 July 2004; accepted 25 September 2004
Abstract
Sludge retention time (SRT) can produce signicant effects on biomass properties in a membrane bioreactor (MBR) system. In this study,
the membrane separation process was coupled to a sequencing batch reactor (SBR), which is one of the biological nutrient removal (BNR)
processes, and the inuence of SRT on membrane fouling and biological activity was investigated. Membrane fouling increased with SRT
since sludge particles were more severely deposited on the membrane surface at longer SRT. Regardless of SRT change, COD removal
efciency was high and stable (over 92%) throughout the experiment. Nitrogen removal efciency also attained a high treatment level.
However, it was not proportioned to SRT increase and rather decreased at the longest SRT. Phosphorus removal decreased at prolonged SRT
since excess sludge was reduced. Biological activity such as specic oxygen uptake rate (SOUR), specic nitrication rate (SNR), and specic
denitrication rate (SDNR) did not increase with SRT but decreased at prolonged SRT.
# 2004 Elsevier Ltd. All rights reserved.
Keywords: Membrane bioreactor (MBR); Sequencing batch reactor (SBR); Membrane fouling; Sludge retention time (SRT); Specic oxygen uptake rate
(SOUR); Specic nitrication rate (SNR); Specic denitrication rate (SDNR)
1. Introduction
It is well known that sludge retention time (SRT) is the
one of the important factors, which can change the state of
biomass in an activated sludge system [1,2] and the con-
centration of mixed liquor suspended solid (MLSS) in the
bioreactor increased with SRT [3]. A membrane bioreactor
(MBR) system can maintain higher MLSS compared to a
conventional activated sludge system through membrane
separation technology, which can accomplish perfect solid/
liquid separation [4]. Therefore, it is not difcult to expect
that biomass properties and membrane fouling in a MBR
system can be signicantly inuenced by SRT. In fact, many
MBR researchers have operated their systems with longer
SRT compared to conventional biological treatment since
they believed that a higher biomass concentration, which
was derived by longer SRT, gave rise to higher treatment
efciency. Some MBR plants were operated with an innite
SRT in order to maintain large amounts of biomass.
However, it is not difcult to expect that treatment efciency
would not be linearly proportioned to biomass concentration
because the specic bioactivity can be reduced at substrate
decient states.
On the other hand, higher MLSS concentrations can
accelerate membrane fouling via rapid deposition of sludge
particles on the membrane surface [5]. Furthermore, it was
reported that properties of mixed liquor, such as viscosity,
amount and composition of microbial product and cell
surface properties were changed at longer SRT [6,7]. These
properties can also inuence membrane fouling. Since
membrane fouling is one of the most important problems of
www.elsevier.com/locate/procbio
Process Biochemistry 40 (2005) 23932400
* Corresponding author. Tel.: +82 2 880 4621; fax: +82 2 873 2285.
E-mail address: tmtak@snu.ac.kr (T.-M. Tak).
0032-9592/$ see front matter # 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.procbio.2004.09.017
MBR processes, the inuence of SRT on membrane fouling
needs to be investigated.
It was reported that adjustment of SRT value is essential
for better biological nutrient removal processes (BNR),
which have attracted great attention for economical nitrogen
and phosphorus removal [8]. Studies on BNR-conducting
MBR systems have been conducted by several researchers in
recent years and there is growing interest on those processes
[911]. Thus, the inuence of longer SRTin MBR system on
BNR performance needs to be claried.
Considering the aspects mentioned above, SRTs have
signicant effects on biological activity and membrane per-
formance in BNR-conducting MBR systems. In this study, a
membrane unit was coupled to a sequencing batch reactor
(SBR), whichis one of the BNRprocesses, andthe systemwas
operated with synthetic wastewater. The main purpose of this
study was to investigate the effect of SRT on specic biolo-
gical activity including BNR performance and membrane
fouling in a membrane coupled sequencing batch reactor.
2. Materials and methods
2.1. Experimental set-up
The experimental set-up is shown in Fig. 1. Four-parallel
reactors were operated simultaneously and controlled by
computer connected to a programmable logic controller
(PLC: LG Industrial System, Korea). U-shape hollow bre
membrane modules were directly submerged in the reactors.
The air diffusers were installed under the membrane module
to optimize the contact between the air bubbles and the
membrane surface. Thus, solid accumulation on the
membrane surface could be prevented by a sheering stress
generated by the uplifting ow of bubbling air. The pressure
gauges were installed in order to monitor the variation of t
he trans-membrane pressure (TMP) between the membranes
and suction pumps. To maintain a constant level in the
reactor, a level sensor was used. Submerged circulation
pumps were used for sludge mixing during the non-aeration
period.
The bioreactor is a rectangular tank of 200 mm
250 mm 350 mm. The membrane module used here was a
hollow bre membrane module made of polyethylene
(Mitsubishi Rayon Engineering Co., Japan) with a pore size
0.4 mm and a ltration area of 0.3 m
2
and the efuent was
sucked out by metering-pump (FMI QD PUMP, USA).
Operating conditions are summarized in Table 1. The four
bioreactors were operated at the same hydraulic residence
time (HRT) and air ow rate. Temperature and pH are
adjusted in order to eliminate their inuences. Since the
the SRT of the reactors were 30, 50, 70 and 100 days
MLSS concentrations were maintained at approximately
(a) 7000 mg/l, (b) 10,000 mg/l, (c) 14,000 mg/l and (d)
18,000 mg/l, respectively. Food to microorganism ratios
(F/M) of all reactors were about 0.060.15 kg COD/kg
MLSS-day. These values are lower range than those of
conventional systems.
S.-S. Han et al. / Process Biochemistry 40 (2005) 23932400 2394
Fig. 1. Schematic diagram of experimental system.
The SBR operation sequence is described in Fig. 2.
Reactor conditions, i.e. anaerobic, anoxic, and anaerobic
condition, were changed during the process time by power
on/off of air blower controlled automatically by PLC.
After the initial 60 min of feeding and anaerobic phase for
phosphorus release, 40 min of aeration was applied to the
reactors for organic decomposition and nitrication. The
reactors then were not aerated but mixed constantly by
submerged circulation pumps for 70 min. During that
period, denitrication could occur after oxygen was con-
sumed. Before the suction period, 30 min of aeration was
applied for removal of residual COD and phosphorus luxury
uptake. During the suction period, the reactor was aerated
and 8 min/2 min intermittent suction was applied in order to
control membrane fouling.
2.2. Synthetic wastewater and microorganism
A synthetic wastewater used for this study contained
glucose, (NH
4
)
2
SO
4
, and KH
2
PO
4
as the sources of carbon,
nitrogen, and phosphorus, respectively. COD, nitrogen and
phosphorus concentrations of inuent were set at 500, 100
and 50 mg/l, respectively. Seeding sludge was supplied from
a nearby sewage treatment plant. After seeding, the sludge
was cultivated with synthetic wastewater over 100 days for
acclimation of microorganisms.
2.3. Membrane performance assessment
First of all, membrane separation characteristics were
investigated. The air scouring effect by air blowing and
critical ux, which can be viewed as the ux at which solid
deposition starts to occur [13], were measured.
Since it was reported that cake formation on membrane
surfaces plays a main role in MBR systems, sludge
deposition on the membranes was calculated quantitatively
using the resistance model [14].
R
DPt
hJ
where R: ltration resistance (m
1
), J: permeation ux
(m
3
/m
2
s), DPt: TMP (Pa), h: viscosity of permeate (Pa s).
Sub-critical ux operation is essential for long time use of
membranes without washing or substitution. It has been
known that irreversible membrane fouling is developed
rapidly beyond the critical ux [15]. This study measured
critical ux by monitoring the ux with ltration time at
constant TMP using a metering pump.
2.4. Analytical method
Standard methods [16] were adopted for the measure-
ment of water quality. Measurement of DO concentration
was carried out with OX22 (AQUA LYTIC, Germany).
COD, total phosphorus (TP) and ortho-phosphate concen-
tration are determined using a spectrophotometric method
with Fotometer AL282 (AQUA LYTIC, Germany) and
reagent kits. Total Kjeldahl nitrogen (TKN) was measured
with a Kjeltec Auto 2300 analyzer (Tecator, Sweden).
Oxidized nitrogen, including the nitrite and nitrate concen-
trations, were determined using ion chromatography
(Shimadzu, Japan).
S.-S. Han et al. / Process Biochemistry 40 (2005) 23932400 2395
Fig. 2. Operation mode of membrane coupled SBR system.
Table 1
Operating conditions of Membrane coupled SBR system
Operating conditions
Working volume (L) 12
Feeding volume (L) 4
Hydraulic retention time (h) 12
Four sludge retention time (days) 30 50 70 100
MLSS concentration (mg/L) 7000 10,000 14,000 18,000
F/M (kg COD/kg MLSS d) 0.15 0.10 0.07 0.05
Aeration intensity (L/min) 15 20 20 25
Dissolved Oxygen (mg/L) 23
Temperature 25 2 8C
pH 7.08.0
2.5. Biological activity measurement
Since oxygen is required for microorganisms to decom-
pose organic compounds in a biological treatment process,
biological activity for COD removal can be characterized by
specic oxygen uptake rates (SOUR). SOURs were
measured using a Winkler bottle method. Hundred milli-
litres synthetic wastewater added to 300 ml sludge sample in
the bottle and the mixed samples were aerated until the DO
reached constant level. Aeration was stopped and DO con-
centration was constantly measured using an oxygen sensor.
During the experiment, samples were constantly stirred
using a magnetic stirrer. The decreases in DO-concentra-
tions were transferred into a utilization rate, assuming
linearity in the decreasing slope. SOUR was calculated by
the following equation:
SOUR (mg O
2
/g MLSS h) = O
2
consumption rate (mg
O
2
/l min) MLSS
1
(l/g) (60 min/h)
For the measurement of nitricationdenitrication
activity, specic nitrication rate (SNR; mg NO
3
N/
g MLSS h) and specic denitrication rate (SDNR; mg
NO
3
N/g MLSS h) batch experiments were conducted [12].
SNR was measured by the following method. Six hundred
millilitres of MLSS solutions was prepared in a ask and
200 ml synthetic wastewater added. The mixed sample was
aerated and samples for NO
3
N analysis obtained at timed
intervals using directly submerged mini membrane modules
made by the authors. SNR was calculated by monitoring the
increased rate of NO
3
N concentration versus times at
aerobic condition. SDNR was measured through the
same procedure of SNR. However synthetic wastewater
for SDNR measurement was prepared using sodium nitrate
as nitrogen source instead of ammonium sulphate. SDNR
was calculated by monitoring the rate of decrease of NO
3
N.
3. Results and discussion
3.1. Membrane performance according to the
ltration condition
A typical MBR process using submerged membranes is
implemented by causing a shearing stress through uplifting
air bubbles. In order to measure the air scouring effect, ux
declines according to air blow intensity were monitored.
Variation of total ltration resistance according to SRT
changes are shown in Fig. 3. This represents the effect of
air ow intensity on membrane fouling in the activated
sludge MBR process. Resistance changes of non-aeration
and aeration condition show that sludge deposition was
signicantly prevented by air ow. The scouring effect was
increased with air ow intensity. However, it was not
linearly proportioned to air ow and there was critical air
ow intensity at which scouring effect hardly improved.
This tendency was reported in our previous studies [11,17].
The existence of critical air ow intensity indicates limit
ow velocity due to the resistance of uid. Air scouring
effect was hardly increased above the 15 l/min of air blow
intensity at SRT 30 days and this trend was also observed at
the other SRTs. As shown in Fig. 3, critical air ow intensity
gradually increased with the increase of SRT due to higher
MLSS concentration and viscosity.
It should be noted that increase of air ow intensity for
fouling control can result in an over-supply of DO and poor
denitrication which is reported as the limiting step for
nitrogen removal in a membrane coupled BNR system [10].
Furthermore, since power consumption increases with air
blow intensity, the operation cost of MBR process increases.
Thus, over aeration for fouling control may cause a
deterioration effect on MBR process. Since oxygen supply
to a reactor is sufcient to maintain aerobic condition, each
reactor was operated at a critical ow intensity in this study
(Table 1).
The concept of critical ux was shown experimentally by
Defrance and Jaffrin [15]. The critical ux is dened as the
ux below which ux decline with time does not occur.
Fig. 4 shows the result of critical ux measurement. At SRT
30 days, ux decline did not occur until the TMP increased
up to 23 K Pa, however, 47 l/m
2
h ux began to decrease
slightly at 27 K Pa. Then, ux decreased more rapidly and
TMP was not controlled consistently at 37 K Pa. Therefore,
it can be concluded that the critical ux of SRT 30 days was
about 47 l/m
2
h. The observed critical ux decreased
according to the increase of SRT, 43 l/m
2
h, 42 l/m
2
h and
36 l/m
2
h were observed at SRT 50, 70 and 100 days,
respectively. Membrane performance studies clearly showed
that membranes are fouled more severely and the control
of membrane fouling with air scour is more difcult at
prolonged SRT.
3.2. Treated water quality
The average treatment efciencies for about 40 days
operation are shown in Fig. 5. As shown in Fig. 5(a), the
COD removal rate slightly increased with SRT due to the
higher concentration of biomass which can decompose
organic compounds. Although COD removal in the
bioreactor slightly decreased with shortened SRT, the total
removal efciency of organic compound could be kept over
92% regardless of SRT. This high and stable COD removal
could be achieved by the maintenance of higher MLSS
concentration compared to conventional system and
membrane separation of macromolecular COD components
which might be generated from microbial metabolism. It
was reported that membrane separation plays an important
role in maintaining high and stable COD removal [18].
The removal efciency for total nitrogen (TN) also
showed a satisfactory level, less than an efuent nitrogen
concentration of 10 mg/l. This is because of the longer
sludge retention times of the nitrifying and the denitrifying
bacteria. However, the treatment efciency was not linearly
proportioned to SRT. It appeared that nitrogen removal of
S.-S. Han et al. / Process Biochemistry 40 (2005) 23932400 2396
SRT 100 days was less than that of SRT 50 and 70 days. This
may be due to the lower growth rate of microorganism and
specic biomass activity.
Since the nitrogen in the reactor could be consumed by
new microbial synthesis, TN removal could be lowered at
extremely prolonged SRT because of lower growing rate.
Specic microbial activity can be inuenced by the amount
of oxygen and substrate available. Organic decomposition
and nitrication, which mainly occurred in aerobic condi-
tions, required sufcient oxygen as electron acceptor.
Although even the DO concentration of the bulk solution
is at a sufcient level to maintain aerobic condition,
inefcient oxygen transfer can be derived by increased uid
resistance due to the high MLSS concentration and viscosity.
Since the substrate decient state, which was generated by
low food to microorganism ratio, gave rise to competition of
biomass, specic bioactivity could be reduced. The effect of
SRT on nitricationdenitrication will be discussed with
experimental evidence in the following section. Since
inefcient oxygen transfer and substrate decient state gave
rise to lowered specic biological activity, it can be
concluded that maintaining appropriate SRT is required
for efcient nitrogen removal.
As shown in Fig. 5(c), inuent total phosphorus (TP)
concentration was very high. Therefore, TP was not well
removed due to the limitation of biological process. The
limitation would be attributed to the fact that removal of
phosphorus ultimately depends on the amount of excess
sludge wasting. Thus, maintaining relatively shorter SRT,
which means a large amount of excess sludge discharge, can
have an advantage for phosphorus removal compared to
maintaining longer SRT.
3.3. In situ nitrication and denitrication analysis
Oxidized nitrogen concentrations of sludge mixed liquor
were monitored during the aerobic and anoxic phases.
Nitrication and denitricaton proles of membrane
coupled SBR systems are shown in Fig. 6. Nitrication
and denitrication performance was improved with increase
of SRT until SRT 70 days since the amount of nitrier and
denitrier increased. Thus, nitrogen removal increased from
87 to 96% as shown in Fig. 5(b). However, nitrogen removal
efciency was decreased to 89% at SRT 100 days. Fig. 6
shows that nitrication rate of SRT 100 days was not
different fromthose of SRT 50 and 70 days but denitricaton
prole was worse than that of shorter SRT. Since the MLSS
concentration increased to about 18,000 mg/l, mass transfer
of electron acceptor and carbon source might be hindered by
great amount of solid matter and increased uid viscosity.
Accumulation of inert matter, which has lower bioavail-
ability, also caused poor denitrication prole.
S.-S. Han et al. / Process Biochemistry 40 (2005) 23932400 2397
Fig. 3. Variation of total ltration resistance according to SRT change (TMP: 15 kPa, temperature: 25 2 8C; a: SRT = 30 days, b: SRT = 50 days, c: SRT = 70
days, d: SRT = 100 days).
S.-S. Han et al. / Process Biochemistry 40 (2005) 23932400 2398
Fig. 4. Variation of critical ux according to SRT change (a: SRT = 30 days, b: SRT = 50 days, c: SRT = 70 days, d: SRT = 100 days).
Fig. 5. COD, TN (total nitrogen is the sum of TKN and NO
x
N) and TP removal behavior according to SRT change (a: COD, b: TNandc:TP).
3.4. Specic sludge activities measurement according to
SRT change
Changes of sludge activities with different SRT are
illustrated in Table 2. With respect to organic decomposi-
tion, SOUR was not inuenced by increase of SRT until
SRT 70 days. However, the biomass of SRT 100 days had a
lower oxygen utilization rate compared to the biomass
of shorter SRT. This might be explained by an impeded
transfer rate of both substrate and oxygen according to
an increase of the sludge viscosity at long SRT and
accumulation of inert matter according to the endogenous
respiration [18].
The nitrifying activity of sludge according to the different
SRT was also investigated. As shown in Table 2, although
there is no big difference between SRT 50 and 70 days, SNR
slightly decreased with increase of SRT. The decrease of the
specic nitrication rate at longer SRT might be due to the
lower oxygen transfer and decient substrate. Although total
nitrication rate slightly increased, specic nitrication rate
decreased by competition of biomass derived from low F/M
ratio. Specic denitrication rate increased with SRT, but
decreased signicantly at extremely prolonged SRT. This
might also be due to the competition of denitrier for
substrate.
As mentioned above, prolonged SRT give rise to
deterioration effects on specic biomass activities. Further-
more, since high viscosity and large amounts of inert matter
can cause severe membrane fouling, extremely prolonged
SRT give adverse effects on MBR performance.
4. Conclusions
Major ndings from this study are summarized as
follows:
(1) The membrane fouling rate increased with SRT,
presumably due to large amount of foulants and high
uid viscosity. Thus, higher air ow intensity was
needed for fouling control at prolonged SRT.
(2) Critical ux decreased with increase of SRT, indicating
that membrane fouling started to occur even at low ux
condition.
(3) COD removal in the bioreactor slightly decreased with
shortened SRT but total removal efciency could be
maintained at over 92% regardless of SRT.
(4) Nitrogen removal was increased with SRT until SRT 70
days. But the removal efciency decreased at SRT 100
days because of low biomass growth and poor denitri-
cation.
(5) Phosphorus removal also showed poor performance at
prolonged SRT since amount of excess sludge reduced.
(6) Specic biological activities such as SOUR, SNR,
SDNR were decreased at prolonged SRT. This might be
explained by impeded transfer rate of both substrate and
oxygen and accumulation of inert biomass due to
endogenous respiration. The ndings of this study show
that prolonged SRT gives rise to deterioration effects on
the process of BNR conducting MBR system in aspects
of membrane fouling and bioactivities. Thus, appro-
priate SRT need to be maintained for efcient operation
of MBR process.
Acknowledgement
The authors are grateful to the Ministry of Science &
Technology, Republic of Korea for their nancial support
under Grant M1-0214-00-0303-03-B15-00-043-10.
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