You are on page 1of 12

See discussions, stats, and author profiles for this publication at: https://www.researchgate.

net/publication/321786827

Effect of powdered activated carbon dosage on sludge properties and


membrane bioreactor performance in a hybrid MBR-PAC system

Article  in  Environmental Technology · December 2017


DOI: 10.1080/09593330.2017.1417493

CITATIONS READS

3 109

5 authors, including:

Shi Zhang Xingtao Zuo


Chinese Academy of Sciences Huazhong Agricultural University
4 PUBLICATIONS   12 CITATIONS    31 PUBLICATIONS   270 CITATIONS   

SEE PROFILE SEE PROFILE

Hu Bo
Czech University of Life Sciences Prague
7 PUBLICATIONS   17 CITATIONS   

SEE PROFILE

Some of the authors of this publication are also working on these related projects:

Effects of arbuscular mycorrhizal fungi(AMF) on the removal of emerging pollutants(EPs) in constructed wetlands View project

algal membrane harvesting View project

All content following this page was uploaded by Shi Zhang on 02 April 2019.

The user has requested enhancement of the downloaded file.


Environmental Technology

ISSN: 0959-3330 (Print) 1479-487X (Online) Journal homepage: https://www.tandfonline.com/loi/tent20

Effect of powdered activated carbon dosage on


sludge properties and membrane bioreactor
performance in a hybrid MBR-PAC system

Shi Zhang, Xingtao Zuo, Juan Xiong, Cong Ma & Bo Hu

To cite this article: Shi Zhang, Xingtao Zuo, Juan Xiong, Cong Ma & Bo Hu (2019) Effect
of powdered activated carbon dosage on sludge properties and membrane bioreactor
performance in a hybrid MBR-PAC system, Environmental Technology, 40:9, 1156-1165, DOI:
10.1080/09593330.2017.1417493

To link to this article: https://doi.org/10.1080/09593330.2017.1417493

Accepted author version posted online: 13


Dec 2017.
Published online: 22 Dec 2017.

Submit your article to this journal

Article views: 82

View Crossmark data

Full Terms & Conditions of access and use can be found at


https://www.tandfonline.com/action/journalInformation?journalCode=tent20
ENVIRONMENTAL TECHNOLOGY
2019, VOL. 40, NO. 9, 1156–1165
https://doi.org/10.1080/09593330.2017.1417493

Effect of powdered activated carbon dosage on sludge properties and membrane


bioreactor performance in a hybrid MBR-PAC system
Shi Zhanga, Xingtao Zuoa, Juan Xiongb, Cong Mac and Bo Hua
a
College of Resources and Environment, Huazhong Agricultural University, Wuhan, People’s Republic of China; bCollege of Science, Huazhong
Agricultural University, Wuhan, People’s Republic of China; cDepartment of Chemical and Biomolecular Engineering, University of Connecticut,
Storrs, CT, USA

ABSTRACT ARTICLE HISTORY


An improved insight into the effect of powdered activated carbon (PAC) on membrane fouling is Received 6 September 2017
crucial to the MBR performance. Sludge key property, soluble microbial products (SMP) and Accepted 10 December 2017
transmembrane pressure (TMP) were monitored. The membrane fouling rate in the MBRs was
KEYWORDS
also analyzed based on TMP profile and resistance-in-series model. PAC reduced the membrane Activated sludge; MBR; PAC;
filtration resistance and significantly decreased the fouling rate. The sludge filterability was SMP; membrane fouling
improved by extending the filtration time by almost twofold. PAC affected the SMP release and
protein/polysaccharide (carbohydrate) was in a lower ratio. Fourier transform infrared (FTIR)
analysis indicated that PAC decreased the impact of organic carbon, and reduced the proteins’
and polysaccharides’ absorption and deposition on the membrane surface and in the pores. The
degree of reversible and irreversible fouling was related to the PAC content added into the
MBRs. At the optimum dosage of 2 g/L, the results signified the PAC potential as a mitigation
strategy of membrane fouling.

1. Introduction
foulants such as soluble extracellular polymeric sub-
MBR technology has been widely used for the treatment stances (EPS) or soluble microbial products (SMP) by
and reclamation of both industrial and municipal waste- PAC; (3) the formation of a more rigid and less compres-
waters. However, membrane fouling is still the main sible cake or gel layer; (4) an improved flocculation. To
drawback impeding the application of MBR technology. further improve this process, a better understanding of
Membrane fouling is mainly affected by membrane the fouling differences in MBR with and without PAC is
properties, operating conditions and solution character- needed [14].
istics. The suspended solids and active microorganisms The 0.3% PAC in MBR reduced trihalo-methane (THM)
in MBR make membrane fouling an inevitable phenom- precursors by over 98% [15]. PAC was effective in redu-
enon [1], and it will increase the membrane cleaning fre- cing the permeation flux loss at a lower dosage of 2–
quency and reduce the membrane lifespan [2]. Many 5 mg/L [16] and 1.67 g/L, but increased the membrane
studies have tried to mitigate membrane fouling by flux at 3.4 g/L PAC [17]. A low PAC dosage of 0.5 g/L com-
introducing fouling reducers into the MBR system, such bined with a relatively long SRT (50 days) extended the
as organic polymer [3] and inorganic materials (alum filtration period without significant fouling at high flux
chloride, zeolite, etc.) [4–6]. However, these methods (72 L/(m2·h) for 18 h and 50 L/(m2·h) for 180 h), and the
failed due to relatively high operating costs. critical flux increased by 10% [13]. Different optimal
Powdered activated carbon (PAC) added into MBR is a dosages of PAC in MBR were obtained for the treatment
more effective and economical technique to mitigate of different feed or wastewater. A 2 g/L PAC performed
membrane fouling [7–10]. This process can reduce the as the best organic matter and for ammonia removal
operation and maintenance costs of membrane cleaning of the micro-polluted surface water [18], 4 g/L for less
and membrane replacement by about 25% [11]. Several dosage cost [10] and 5 g/L for higher pollutants
mechanisms were employed to explain this positive removal efficiencies and stability against shock loading
effect [12–14]: (1) enhanced scouring of the membrane [19]. Even at a higher PAC dosage of 40–50 g/L, the
surface to avoid particle deposition; (2) adsorption of membrane fouling frequency was lower [20].

CONTACT Xingtao Zuo xingtaozuo@aliyun.com College of Resources and Environment, Huazhong Agricultural University, Wuhan, People’s Republic of
China; Juan Xiong xiong@mail.hzau.edu.cn College of Science, Huazhong Agricultural University, Wuhan, People’s Republic of China
Supplemental data for this article can be accessed at https://doi.org/10.1080/09593330.2017.1417493
© 2017 Informa UK Limited, trading as Taylor & Francis Group
ENVIRONMENTAL TECHNOLOGY 1157

SMP and EPS are composed of a variety of organic on and 2 min off. Transmembrane pressure (TMP) was
compounds released from microorganisms due to their continuously monitored online using a high-resolution
metabolic activity [21], which are considered to be (0.1 kPa) pressure sensor which was connected to a per-
major foulants in MBRs [22]. However, limited research sonal computer for data recording. The schematic of
has reported the effect of different PAC dosages on MBR is shown in Figure 1.
SMP. Zhao and Gu [23] found that PAC could effectively PAC used in this work was wood charcoal with the
reduce the EPS content and significantly decrease the particle size of 200 mesh. PAC was dried at 105°C for
irreversible membrane fouling when PAC was 0.75 g/L, 1 h and cooled down at 25°C inside a desiccator before
but the effect was dramatically reduced at a higher con- use. Then, PAC was added directly into the reactor to
centration of 1.5 g/L. In a similar study, 2 g/L of PAC obtain a PAC concentration of 0, 1, 2 and 4 g/L, which
addition had little effect on EPS concentration, but the was labeled as MBR-control and MBR-PAC (1, 2 and
proteins/carbohydrates ratio in SMPs was high and 4 g/L), respectively. There was no further addition of
Sludge Volume Index (SVI) decreased, which improved PAC into the system.
sludge dewaterability [24].
The objective of this study was to provide additional
2.2. Extraction of foulants
insight into the effects of PAC addition on membrane
fouling mitigation. The dynamics characteristics of acti- At the end of the membrane operation cycle when TMP
vated sludge were simultaneously monitored in four par- reached 40 kPa, the fouled membrane module was
allel lab-scale MBRs during the continuous operation removed and washed using the following procedures
period (157 days) without sludge discharge. Specifically, [9,22]: (i)The fouled membrane module was washed
SMP variation caused by different PAC concentrations in with Milli-Q water, and then wiped the foulants from
MBRs was investigated. The foulant extracted from the the membrane surface with a sponge followed by
fouled membranes in the cleaning procedure at the washed with Milli-Q water. The washing solution was col-
end of the membrane operation cycle was characterized lected and froze-dried. The pure water flux of the mem-
to confirm the effects of PAC on the foulants. This knowl- branes cleaned with water was measured. (ii) After
edge can be used to fine-tune the PAC dosage and to physical cleaning, the membrane was chemically
assess the possibility of applying a fouling reducer. cleaned by soaking in 0.01 mol/L NaOH, and then
0.1 wt% sodium citrate for 24 h. The washing solution
was collected separately and then filtered using a
2. Materials and methods 0.45 μm membrane followed by freeze drying. After
each step of chemical cleaning, the membrane
2.1. Experimental set-up and operation
modules were rinsed completely with Milli-Q water.
Four identical lab-scale MBRs with a volume of 22 L were Then, the corresponding pure water fluxes of the mem-
continuously operated in parallel and fed with synthetic brane module were measured.
wastewater for 157 days. The composition of the synthetic
wastewater is given as follows: glucose 344 mg/L, urea
2.3. Analytical methods
33 mg/L, (NH4)2SO4 120 mg/L, KH2PO4 15 mg/L, K2HPO4
20 mg/L, MgSO4·7H2O 24.4 mg/L, CaCl2·2H2O 12 mg/L, COD, NH+ 4 − N, TN, VSS and MLSS were measured
FeCl3·7H2O 1.5 mg/L, ZnSO4·7H2O 0.15 mg/L, CuSO4·5H2- according to the standard methods [25]. TOC was
O 0.05 mg/L, Pb(NO3)2 0.26 mg/L, and adding NaHCO3 measured by a Shimadzu analyzer. Polysaccharides and
to adjust the pH value. COD was 398 mg/L on average proteins were quantified in SMP samples filtered with
but fluctuated between 320 and 480 mg/L. NH+ 4 −N 0.45 μm membrane. Polysaccharides concentrations
and TN concentrations were 38.6 ± 4.9 mg/L and 63.0 ± were determined spectrophotometrically with phenol-
7.0 mg/L, respectively. The inoculated activated sludge sulfuric acid employing glucose as the standard [26].
was obtained from the local municipal wastewater treat- Protein concentrations were determined with the
ment plant. Lowry method [27] using bovine serum albumin as the
Each MBR contained a submerged PVDF hollow fiber standard.
membrane module with a nominal pore size of 0.2 μm The resistance analysis was measured by applying
and an effective filtration area of 0.3 m2 (MOF-1B-W, resistance-in-series model to evaluate the membrane fil-
MOTECH, China). The oxygen concentration in the tank tration characteristics [8,23,28]. Fourier transform infra-
was measured online and controlled at 2–4 mg/L. The red spectroscopy (FTIR) was used to investigate the
overall HRT was 6 h. The permeate pump was operated structural information of the foulants extracted from
in an intermittent suction mode with a cycle of 8 min the membrane module.
1158 S. ZHANG ET AL.

Figure 1. Schematic diagram of MBR.

3. Results and discussion ammonia removal. The higher specific surface of PAC
was favorable for the nitrifying bacterial to proliferate,
3.1. COD, NH+
4 − N and TN removal thus enhancing their biological reaction rate [20]. In
Figure 2 shows the removal efficiencies of COD in MBR addition, the ammonia nitrogen content of the super-
with and without PAC. There was no significant differ- natant was almost the same as the effluent for all MBRs
ence in COD removal rate for the four studied systems, systems. That was explained by that ammonia nitrogen
i.e. no discernible increase in COD removal before and existed in the form of hydrated ammonia ions in water,
after addition of PAC. Average COD removal rates of and it could free cross through the membrane pores.
the supernatants were 92.44%⍰92.86% and 92.22% of The removal of TN was also monitored (see support-
MBR-PAC with 1, 2 and 4 g/L compared with 92.02% ing materials Figure S2 and Figure S3). The average
of MBR-control. Their corresponding total removal rates removal rates were 40.38%, 38.80%, 38.55% and
were 95.35%, 95.41%, 95.01% and 94.26%, respectively. 37.44% for MBR without and with PAC content of 1, 2
This result indicated that the addition of PAC had a and 4 g/L, respectively. The MBR in this work contained
weak but positive effect on COD removal. It is worth no anoxic zone to support simultaneous nitrification
noting that in the MBR-PAC (2 g/L) system, both the and denitrification. This is consistent with other works
supernatant and effluent got best removal efficiency, [8,30], who found no discernible increase in TN
which had good interception and degradation effect removal after addition of PAC.
on the soluble molecules in water and kept the effluent
quality stable [29]. Hu et al. [18] also found that 2 g/L of
3.2. MLSS, MLVSS/MLSS and SVI
PAC was more conducive to COD removal. This was
similar to the observation of Zhao and Gu [23], who The variation of MLSS and MLVSS concentration in the
reported that a dosage of 1.5 g/L PAC added in MBR four MBRs are shown in Figure 3. An estimated 4 g/L
resulted in the highest removal rate of the supernatant PAC added into MBR resulted in a more considerable
COD in the early stage of operation. increment in MLSS concentration in the initial 0–40
Average NH+ 4 − N removal rates of the supernatants days than those of the lower PAC concentrations of 0,
were 98.59%, 98.89% and 97.63% for MBR-PAC with 1, 1 and 2 g/L. Also, at the same period, no significant
2 and 4 g/L PAC compared with 94.82% of MBR- changes in MLSS concentration were observed
control, respectively (see supporting materials Figure between MBR-control and MBR-PAC (1 and 2 g/L)
S1). The corresponding NH+ 4 − N removal rates were systems. This again meant that higher PAC dosage was
94.19%, 98.81%, 98.89% and 97.08% as PAC dosage more conducive to promote rapid propagation of micro-
increased. The NH+ 4 − N removal efficiency of the MBR organism. MLSS concentrations of MBR-PAC systems
in the presence of PAC was higher than that of MBR- were higher than MBR-control in the later 90–147 days.
control. The increased degree of NH+ 4 − N removal was PAC helped in microbial growth due to the increase in
similar at 1 g/L and 2 g/L of PAC. The result also an available surface area [31,32]. The MLSS concentration
suggested that PAC addition increased NH+ 4 −N of the MBR-PAC systems maintained at 15–17 g/L in the
removal rate but much higher dosage could not later 125–147 days.
improve its removal efficiency. Compared to organic MLVSS/MLSS increased in all MBRs, showing that the
matter removal (COD), PAC addition was beneficial to sludge activity improved during long-term operation,
ENVIRONMENTAL TECHNOLOGY 1159

Figure 2. Variation of COD in the MBRs: (a) MBR-control, (b) MBR-PAC(1 g/L), (c) MBR-PAC(2 g/L) and (d) MBR-PAC(4 g/L).

and the growth and reproduction of microorganisms treatment plant [34], illustrating that in this work, the
also increased [33]. There was no remarkable difference reactors were in a relatively stable operation state.
observed in MLVSS/MLSS values of all the MBRs. It is clear from Figure 4 that SVI showed a sharp
However, the MLVSS/MLSS of MBR-control was slightly increase in the initial operation stage of MBR-control
higher than MBR-PAC systems until the 120th day, system. While SVI of MBR-PAC systems presented a
meaning that PAC addition did not lead to the increase gradual increase, suggesting that addition of PAC miti-
in MLVSS/MLSS ratio. Even in the later 140–167 days, gated the SVI increment. The temperature was above
the MLVSS/MLSS of the MBRs was also close. The 30°C in the initial 0–45 days, resulting in increased SVI fol-
average values of MLVSS/MLSS were 0.74–0.78, which lowed by a decrease due to the increased temperature
were close to the value of 0.75 in urban sewage [35]. Also, high SVI was normally attributed to the
growth of filamentous bacteria [32], which was

Figure 3. Variation of MLSS and MLVSS/MLSS versus time. Figure 4. SVI in MBR-control and MBR-PAC systems.
1160 S. ZHANG ET AL.

confirmed by the presence of filamentous fungi in differ- 120 mL/g during the whole operation period, respect-
ent levels observed by microscopic examination of ively. Thus, PAC addition could improve the sludge
sludge in this period (see supporting materials Figure settling properties. The better settleability may be attrib-
S4). After 63 days of operation, the SVI decreased signifi- uted to the role of PAC in promoting colloid and small
cantly even at a high biomass concentration. SVI stabil- particles’ coagulation to form bigger particles [36],
ized below 100 mL/g in the later 127–147 days. This which would enhance strong sludge flocs [37] and/or
revealed that the dependence of SVI on MLSS in the incompressible flocs’ formation [38].
initial and later phases of MBR with and without PAC.
SVI values of all MBRs in this work were always below
3.3. SMP
140 mL/g. The SVI of MBR-PAC systems was lower than
MBR-control. Especially, 2 and 4 g/L of PAC resulted Figure 5(a) presents the SMP concentration in the MBRs.
in lower SVI values, which were less than 100 mL/g and SMP decreased from 9.75 to 7.93 mg/gMLSS in the MBR-
control system during the initial 15 days. Thereafter, SMP
increased to about 10 mg/gMLSS in 45–60 days, and
then decreased in the later 60–147 days. The value fluc-
tuated between 4.55 and 6.55 mg/gMLSS during the
later period. The SMP of MBR-PAC systems decreased
and the variation was marginal with values ranging
from 8.3 to 9.0 mg/gMLSS and 5.1–5.7 mg/gMLSS for
MBR-PAC (1 g/L) and MBR-PAC (4 g/L) in the initial 45
days, respectively. The SMP of MBR-PAC (2 g/L)
decreased by 50% from 11.9 to 5.6 mg/gMLSS in the
same period. Then, the SMP of MBR-PAC systems
increased slightly followed by a decrement in the later
60–147 days.
There was a difference in SMP content in MBR-control
and MBR-PAC systems. The SMP of MBR-PAC systems
was lower than that of MBR-control. SMP decreased by
62.2%, 69.4% and 50.65% in MBRs with PAC of 1, 2 and
4 g/L, respectively. 2 g/L PAC resulted in considerably
lower SMP. These results suggested that PAC addition
could affect the SMP concentration. Damayanti et al.
[5] have also found that the removal rate of SMP in
MBR with PAC was 58%, and demonstrated that PAC
had a good effect on SMP removal. The PAC adsorbed
higher numbers of bacteria [9], and therefore, enhanced
biodegradation was likely to have taken place in the
MBR-PAC system [14].

3.4. Protein/carbohydrate (polysaccharide) ratio


Figure 5(b) presents the protein and polysaccharide con-
centration in the MBRs. The protein and polysaccharide
concentration in SMP did not display a clear trend, and
the variation of them was erratic with sharp fluctuation.
However, the average concentration of protein in the
supernatant were 22.02, 20.75, 17.42 and 20.01 mg/L
for MBR with PAC of 0, 1, 2 and 4 g/L, respectively, and
the corresponding average contents of polysaccharide
were 10.43, 9.75, 8.45, and 9.43 mg/L, respectively.
MBR-PAC (2 g/L) system had the lowest protein and poly-
Figure 5. (a) SMP in the MBRs, (b) Protein and polysaccharide in saccharide content in SMP. The protein and polysacchar-
SMP and (c) P/C ratio in SMP. ide in SMP in the MBR-PAC system were slightly lower
ENVIRONMENTAL TECHNOLOGY 1161

than that of MBR-control. This can be explained by the 3.5. TMP profile
attached growth of biomass on PAC, resulting in the
Under constant flow conditions, the local flux of the
lower synthesis of protein and polysaccharides, and
membrane modules increased, while the TMP increased
SMP adsorbed on PAC.
slowly. When the membrane fouling reached a certain
Many studies have shown that polysaccharides in SMP
extent, the filtration area decreased due to the fouling
are more likely to cause membrane fouling than proteins,
and an increase in local flux, resulting in the pollutants
and it was responsible for the evolution of irreversible
forming cake layers rapidly in the region and it urged
fouling [28,37]. The fouling rate of SMP was positively
TMP to increase suddenly [38].Thus, TMP is a significant
correlated with the polysaccharides’ content [32,39].
parameter for MBR fouling prediction [8]. The influences
This implied that in this work, the SMP in the MBR-PAC
of PAC on the TMP profiles of the MBRs during the first
system had a lower fouling potential, which was also
and second cycle are shown in Figure 6. TMP approach-
indicated in TMP profiles that would be discussed in
ing 50 kPa was set in the first cycle, and 40 kPa in the fol-
the following section. The results were similar to the
lowing operation cycles.
observation of Satyawali and Balakrishnan [32], who
A continuous increase in TMP value was caused by
found that the addition of PAC in MBR resulted in a
fouling formation in/on the membrane during the fil-
decline in both protein and polysaccharide concen-
tration process. Compared with MBR-control system,
tration in SMP.
the time was 78, 84 and 63 d of filtration period for
The protein-to-polysaccharide (P/C) ratio for the MBRs
MBR-PAC (1, 2 and 4 g/L) in the first cycle, respectively.
is shown in Figure 5(c). It is clear that protein was the
The improvement in filterability was obtained in the
dominant component in the SMP from all the MBRs as
MBR-PAC systems by extending the filtration time by
also indicated in Figure 4(b). The average P/C ratio was
almost twofold, signifying the positive effect of PAC on
2.79, 2.60, 2.30 and 2.67 for MBR-control and MBR-PAC
prolonging the MBR operation. Nguyen et al. [30]
with 1, 2 and 4 g/L of PAC, respectively. The P/C ratio
found that the variation in TMP was not significant
was consistently lower in the MBR-PAC system, and the
before and after PAC addition. Other works reported
lowest ratio was obtained in MBR-PAC (2 g/L). Satyawali
that the addition of PAC into MBR did not improve mem-
and Balakrishnan et al. [32] reported that the P/C ratio
brane performance [40] but could rather promote mem-
of the reactor with 2 g/L PAC was higher than that
brane fouling [23,41]. The mechanisms to alleviate
without PAC, and suggested that high P/C ratio improved
membrane fouling included the adsorption of mem-
settleability due to hydrophobic nature of the protein.
brane foulants on PAC, scouring action of PAC, changing
However, in this work, the low P/C ratio seemed to
the composition and permeability of the cake layer and
exhibit better settleability, which correlated well with
improving flocculation of MLSS [12,36,37]. Much lower
the lower SVI values. In addition, the affinity between
SMP content in MBR-PAC systems could also interpret
proteins and foulants should generally be greater than
the difference of TMP [10].
that between polysaccharides and flocs in relation to
In order to better understand the fouling rate of the
their hydrophobicity and surface charge; thus, much
four MBR systems, the membrane fouling rate K was
more proteins were found in the reactors [14].
obtained as ΔTMP/(JΔt). The TMP profiles seemed to
exhibit two stages of fouling, the rapid increase followed
by a steep TMP rise. The two phases of the K values in the
first and second cycle are listed in Table 1. The K1 values
for all the MBR systems were less than K2, suggesting the
fouling rate in the later stage of MBR was higher than
that in the early stage. Especially, the fouling rate of
MBR-PAC system was slower than that in MBR-control

Table 1. Fouling rate of operation cycles in the MBRs.


First cycle Second cycle
MBR PAC (g/L) K1 K2 K K1 K2 K
MBR-control 0 1.55 6.18 3.87 1.16 6.83 3.97
MBR-PAC 1 0.92 4.00 2.46 1.19 5.76 3.47
2 0.98 3.73 2.37 1.09 5.57 3.33
4 1.16 5.16 3.16 1.02 6.35 3.69
Figure 6. TMP variation in the MBRs. Note: K1, slow phase; K2, rapid phase and K, average value.
1162 S. ZHANG ET AL.

system in each stage. PAC addition can be a good control polysaccharides (−1130 cm−1), C–H of aromatic amino
of the increase in TMP. Meanwhile, the K values of MBR- acids and nucleotides (600–660 cm−1) [46]. Band inten-
PAC (2 g/L) were the smallest one among the four MBRs, sity indicated that the quantity of functional groups is
indicating that PAC loading of 2 g/L was found to be suit- responsible for infrared spectroscopy (IR) absorption for
able in membrane fouling mitigation. each frequency. MBR-control and MBR-PAC (4 g/L) pre-
sented the greater intensity for the above-mentioned
bands, which would be expected considering the
3.6. Resistance analysis higher content of the contaminants [47]. The results
The resistance analysis results are summarized in Table 2. revealed that PAC addition reduced the contaminants’
MBR-PAC showed a lower total resistance compared to adsorption and deposition in the cake layer on the mem-
MBR-control. Cake resistance was the main component brane surface. However, a higher dosage of PAC resulted
of the total hydraulic resistance (Rt), having much in contaminants adsorbed on the PAC would be easier to
higher value compared to membrane and pore blocking deposit on the membrane surface [23].
resistance. Hence, the total fouling resistance was more There were clear differences between the peaks as
or less a function of the cake resistance. In addition, shown in Figure 7(a,b). A peak around 2978 and
the membranes suffered from low levels of irreversible 1442 cm−1 suggested the dominance of humic acids
fouling (Rf). Moreover, the cake resistance decreased [44,48]. The observed peaks at around 2496 cm−1
with an increase in PAC concentration. The results indi- (881 cm−1), 1774 and 1006 cm−1 were attributed to car-
cated that the reduction in total resistance was mainly bonates in calcite, silicates and phosphates, respectively
due to the decrease in cake resistance. The incorporation [47]. It is inferred that the humic matters and inorganic
of PAC in MBR could be responsible for the reduction in salts made the main contribution to irreversible mem-
cake resistance [42], as it formed an incompressible par- brane fouling that should be cleaned by NaOH. It
ticular layer of high fluid permeability [12]. should be noted the increase in the relative intensities
It is reported that PAC could help not only reduce the of the bands revealed that PAC increased the irreversible
cake fouling but also prevent pore blocking [8,43]. The membrane fouling in terms of humic matters and the
irreversible fouling resistance was slightly higher in inorganic salts.
the MBR-PAC system when compared to MBR-control. As can be seen from Figure 7(c) in the main bands of
The explanation of this result may be that at a higher contaminants extracted with 0.1% sodium citrate, there
PAC dosage, there was a more serious biofouling [23] were C=O groups of carboxylic acids, esters, ketones
and increased pore blocking by particles in the size and aldehydes (1750–1700 cm−1), C=C of humic
range of the membrane pores [7]. In addition, MBR-PAC matters (1430 cm−1) [49]. The peaks around 1200–
(2 g/L) exhibited the lowest fouling resistance and irre- 900 cm−1 were assigned to carbohydrates and nucleic
versible resistance. acids [46,48]. The peak at 1140 cm−1 was attributed to
polysaccharides. The fingerprint region between 900
and 600 cm−1 exhibited ring vibration from aromatic
3.7. FTIR investigation for foulants amino acids and nucleotides [46]. This meant that poly-
saccharides, aromatic matters, nucleic acids and low mol-
Figure 7(a) shows the FTIR spectra of the foulants
ecular weight organics (carboxylic acids, esters, ketones
extracted by water from the fouled membranes of the
and aldehydes) induced the irreversible fouling that
four MBRs. The main bands identified from the contami-
should be cleaned by sodium citrate. It is clear from
nants in the cake layers corresponded to – OH groups of
the relative intensities of the bands that PAC could also
organic matter (3420 cm−1) C–O of proteins (amide I)
reduce significantly the membrane fouling caused by
(1635 cm−1) [44], nitrate (−1386 cm−1) [45], C–O of
these foulants. In addition, polysaccharide did not
cause significant effects on the irreversible fouling in
the PAC hybrid MBR as indicated in Figure 7(b), and it
Table 2. Filtration resistance in MBR-PAC with different addition
of PAC. may be due to the lower content of them in the
MBR-PAC/ (g/L) reactor. This is in accordance with the result of Khan
Resistance 0 1 2 4 et al. [14].
Total resistance (Rt, 1012m−1) 18.25 17.88 16.37 17.39
Membrane resistance (Rm, 1012m−1) 0.40 0.41 0.40 0.39
Cake resistance (Rc, 1012 m−1) 15.75 14.32 13.16 12.79 4. Conclusions
Irreversible fouling resistance (Rf, 1012 m−1) 2.10 3.15 2.81 4.21
Rc/Rt 86.30 80.09 80.39 73.55 With the addition of PAC, MBR systems achieved a stable
Rf/Rt 11.51 17.62 17.17 24.21
removal efficiency: 95% for COD and 98% forNH+ 4 − N.
ENVIRONMENTAL TECHNOLOGY 1163

Figure 7. FTIR spectra of membrane pollutants: (a) extracted cake layers by water, (b) extracted foulants by 0.01 mol/L NaOH, (c)
extracted foulants by 0.1 wt% sodium citrate.

Compared with the control MBR, SMP release decreased References


by 50–70% and P/C ratio slightly decreased. The cake
[1] Iorhemen OT, Hamza RA, Tay JH. Membrane fouling
resistance as the predominant resistance fraction control in membrane bioreactors (MBRs) using granular
reduced by 18.80% as PAC dosage increased to 4 g/L. materials. Bioresour Technol. 2017;240:9–24.
Polysaccharides did not cause any significant effects on [2] Díaz O, González E, Vera L, et al. Fouling analysis and miti-
the irreversible fouling. The increased irreversible gation in a tertiary MBR operated under restricted aera-
tion. J Membrane Sci. 2017;525:368–377.
fouling after PAC addition may be attributed to humic
[3] Iversen V, Koseoglu H, Yigit NO, et al. Impacts of mem-
substances and inorganic salts. PAC reduced the cake brane flux enhancers on activated sludge respiration
layer accumulation and decreased pore blocking, and and nutrient removal in MBRs. Water Res. 2009;43:822–
thereby mitigated the membrane fouling rate and 830.
extended the filtration period. PAC as an effective [4] Gkotsis PK, Mitrakas MM, Tolkou AK, et al. Batch and con-
fouling reducer with the optimum dosage of 2 g/L exhib- tinuous dosing of conventional and composite coagu-
lation agents for fouling control in a pilot-scale MBR.
ited improved sludge properties and enhanced mem-
Chem Eng J. 2017;311:255–264.
brane performance. [5] Damayanti A, Ujang Z, Salim MR. The influenced of PAC,
zeolite, and moringa oleifera as biofouling reducer (BFR)
on hybrid membrane bioreactor of palm oil mill effluent
Disclosure statement (POME). Bioresour Technol. 2011;102:4341–4346.
[6] Lee JC, Kim JS, Kang IJ, et al. Potential and limitations of
No potential conflict of interest was reported by the authors.
alum or zeolite addition to improve the performance of
a submerged membrane bioreactor. Water Sci Technol.
Funding 2001;43:59–66.
[7] De TL, Maere T, Temmink H, et al. Salt stress in a mem-
This work was supported by Hubei Provincial Natural Science brane bioreactor: dynamics of sludge properties, mem-
Foundation (No. 2016CFB495), and the Fundamental Research brane fouling and remediation through powdered
Funds for the Central Universities (No. 2662017JC019). activated carbon dosing. Water Res. 2014;63:112–124.
1164 S. ZHANG ET AL.

[8] Woo YC, Lee JJ, Shim WG, et al. Effect of powdered acti- [24] Satyawali Y, Balakrishnan M. Performance enhancement
vated carbon on integrated submerged membrane bio- with powdered activated carbon (PAC) addition in a mem-
reactor-nanofiltration process for wastewater brane bioreactor (MBR) treating distillery effluent. J
reclamation. Bioresour Technol. 2016;210:18–25. Hazard Mater. 2009;170:457–465.
[9] Khan MMT, Takizawa S, Lewandowski Z, et al. Membrane [25] APHA. Standard methods for the examination of water
fouling due to dynamic particle size changes in the and wastewater. 20th ed.Washington (DC): American
aerated hybrid PAC–MF system. J Membrane Sci. Public Health Association; 1998.
2011;371:99–107. [26] Dubois M, Gilles KA, Hamilton JK, et al. Colorimetric
[10] Jia S, Han H, Hou B, et al. Treatment of coal gasification method for determination of sugars and related sub-
wastewater by membrane bioreactor hybrid powdered stances. Anal Chem. 1956;28:350–356.
activated carbon (MBR–PAC) system. Chemosphere [27] Lowry OH, Rosebrough NJ, Farr AL, et al. Protein measure-
2014;117:753–759. ment with the folin phenol reagent. J Bio Chem.
[11] Yang W, Paetkau M, Cicek N. Improving the performance 1951;193:265–275.
of membrane bioreactors by powdered activated carbon [28] Ng CA, Sun D, Bashir MJ, et al. Optimization of membrane
dosing with cost considerations. Water Sci Technol. bioreactors by the addition of powdered activated
2010;62:172–179. carbon. Bioresour Technol. 2013;138:38–47.
[12] Jamal KS, Visvanathan C, Jegatheesan V. Effect of pow- [29] Chang IS, Bag SO, Lee CH. Effects of membrane fouling on
dered activated carbon (PAC) and cationic polymer on solute rejection during membrane filtration of activated
biofouling mitigation in hybrid MBRs. Bioresour Technol. sludge. Process Biochem 2001;36:855–860.
2012;113:165–168. [30] Nguyen LN, Hai FI, Long DN, et al. Enhancement of
[13] Remy M, Marel PVD, Zwijnenburg A, et al. Low dose pow- removal of trace organic contaminants by powdered acti-
dered activated carbon addition at high sludge retention vated carbon dosing into membrane bioreactors. J Taiwan
times to reduce fouling in membrane bioreactors. Water Inst Chem E. 2014;45:571–578.
Res 2009;43:345–350. [31] Guo W, Vigneswaran S, Ngo HH, et al. Comparison of the
[14] Khan MM, Takizawa S, Lewandowski Z, et al. Combined performance of submerged membrane bioreactor (SMBR)
effects of EPS and HRT enhanced biofouling on a sub- and submerged membrane adsorption bioreactor
merged and hybrid PAC-MF membrane bioreactor. (SMABR). Bioresour Technol. 2008;99:1012–1017.
Water Res 2013;47:747–757. [32] Satyawali Y, Balakrishnan M. Effect of PAC addition on
[15] Williams MD, Pirbazari M. Membrane bioreactor process sludge properties in an MBR treating high strength waste-
for removing biodegradable organic matter from water. water. Water Res. 2009;43:1577–1588.
Water Res 2007;41:3880–3893. [33] Fan J, Ji F, Xu X, et al. Prediction of the effect of fine grit on
[16] Torretta V, Urbini G, Raboni M, et al. Effect of powdered the MLVSS/MLSS ratio of activated sludge. Bioresour
activated carbon to reduce fouling in membrane bio- Technol. 2015;190:51–56.
reactors: A sustainable solution. case study. Case Study. [34] Wentzel MC, Ubisi MF, Lakay MT, et al. Incorporation of
Sustainability. 2013;5:1501–1509. inorganic material in anoxic/aerobic-activated sludge
[17] Akram A, Stuckey DC. Flux and performance improvement system mixed liquor. Water Res. 2002;36:5074–5082.
in a submerged anaerobic membrane bioreactor (SAMBR) [35] Zhang S, Yang F, Liu Y, et al. Performance of a metallic
using powdered activated carbon (PAC). Process Biochem membrane bioreactor treating simulated distillery waste-
2008;43:93–102. water at temperatures of 30 to 45°C. Desalination.
[18] Hu J, Shang R, Deng H, et al. Effect of PAC dosage in a 2006;194:146–155.
pilot-scale PAC-MBR treating micro-polluted surface [36] Hasan SW, Elektorowicz M, Oleszkiewicz JA. Correlations
water. Bioresour Technol. 2014;154:290–296. between trans-membrane pressure (TMP) and sludge
[19] Park H, Choo KH, Lee CH. Flux enhancement with pow- properties in submerged membrane electro-bioreactor
dered activated carbon addition in the membrane (SMEBR) and conventional membrane bioreactor (MBR).
anaerobic bioreactor. Sep Sci Technol. 1999;34:2781– Bioresour Technol. 2012;120:199–205.
2792. [37] Remy M, Potier V, Temmink H, et al. Why low powdered
[20] Ma C, Yu S, Shi W, et al. Effect of different temperatures on activated carbon addition reduces membrane fouling in
performance and membrane fouling in high concen- MBRs. Water Res. 2010;44:861–867.
tration PAC-MBR system treating micro-polluted surface [38] Kim JS, Lee CH, Chun HD. Comparison of ultrafiltration
water. Bioresour Technol. 2013;141:19–24. characteristics between activated sludge and BAC
[21] Barker DJ, Stuckey DC. A review of soluble microbial pro- sludge. Water Res. 1998;32:3443–3451.
ducts (SMP) in wastewater treatment systems. Water Res [39] Rosenberger S, Laabs C, Lesjean B, et al. Impact of colloidal
1999;33:3063–3082. and soluble organic material on membrane performance
[22] Kimura K, Naruse T, Watanabe Y. Changes in character- in membrane bioreactors for municipal wastewater treat-
istics of soluble microbial products in membrane bio- ment. Water Res. 2006;40:710–720.
reactors associated with different solid retention times: [40] Hai FI, Yamamoto K, Nakajima F, et al. Removal of structu-
relation to membrane fouling. Water Res 2009;43:1033– rally different dyes in submerged membrane fungi reactor
1039. —biosorption/PAC-adsorption, membrane retention and
[23] Zhao Y, Gu P. Effect of powdered activated carbon dosage biodegradation. J Membrane Sci. 2008;325:395–403.
on retarding membrane fouling in MBR. Sep Purif Technol. [41] Ravindran V, Tsai HH, Williams MD, et al. Hybrid mem-
2006;52:154–160. brane bioreactor technology for small water treatment
ENVIRONMENTAL TECHNOLOGY 1165

utilities: process evaluation and primordial considerations. [46] Badireddy AR, Chellam S, Gassman PL, et al. Role of extra-
J Membrane Sci. 2009;344:39–54. cellular polymeric substances in bioflocculation of acti-
[42] Gai XJ, Kim HS. The role of powdered activated carbon in vated sludge microorganisms under glucose-controlled
enhancing the performance of membrane systems for conditions. Water Res. 2010;44:4505–4516.
water treatment. Desalination. 2008;225:288–300. [47] Parolo ME, Savini MC, Loewy RM. Characterization of soil
[43] Skouteris G, Saroj D, Melidis P, et al. The effect of activated organic matter by FT-IR spectroscopy and its relationship
carbon addition on membrane bioreactor processes for with chlorpyrifos sorption. J Environ Manage.
wastewater treatment and reclamation - A critical 2017;196:316–322.
review. Bioresour Technol. 2015;185:399–410. [48] Kimura K, Ogyu R, Miyoshi T, et al. Transition of major com-
[44] Filip Z, Pecher W, Berthelin J. Microbial utilization and ponents in irreversible fouling of MBRs treating municipal
transformation of humic acid-like substances extracted wastewater. Sep Purif Technol. 2015;142:326–331.
from a mixture of municipal refuse and sewage sludge [49] Fels LE, Zamama M, Asli AE, et al. Assessment of biotrans-
disposed of in a landfill. Environ Pollut. 2000;109:83–89. formation of organic matter during co-composting of
[45] Grube M, Lin JG, Lee PH, et al. Evaluation of sewage sewage sludge-lignocelullosic waste by chemical, FTIR
sludge-based compost by FT-IR spectroscopy. analyses, and phytotoxicity tests. Int Biodeter Biodegr.
Geoderma. 2006;130:324–333. 2014;87:128–137.

View publication stats

You might also like