KSCE Journal of Civil Engineering (2014) 18(4):956-963 Environmental Engineering

Copyright ⓒ2014 Korean Society of Civil Engineers

DOI 10.1007/s12205-014-0070-9 pISSN 1226-7988, eISSN 1976-3808
www.springer.com/12205
TECHNICAL NOTE

Implementing Chemical Precipitation as a Pretreatment for Phosphorus Removal

in Membrane Bioreactor-Based Municipal Wastewater Treatment Plants
Jong-Oh Kim* and Jinwook Chung**
Received February 1, 2013/Accepted April 26, 2013

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Abstract

Chemical pretreatment prior to biological treatment is required for achieving wastewater reuse economically by a Membrane
Bioreactor (MBR) and has significant potential in establishing a compact primary settling tank and a secondary biological treatment
system. The purpose of this study was to investigate the factors that affect chemical phosphorus removal as a pretreatment for MBR-
based municipal wastewater. Total Phosphorus (TP) removal from raw wastewater by ferric chloride was more effective compared
with Polyaluminum Chloride (PAC), but PAC was superior to ferric chloride for filtered wastewater. TP removal and Suspended
Solids (SS) removal correlated significantly, unlike TP removal and Total Nitrogen (TN) removal. The optimal pH values for TP
removal was 6.5 and the overall removal efficiencies of TOC and TP were slightly lower compared with turbidity and color removal.
Mixing had little effect on the removal of SS, TOC, turbidity, and color. Conclusively, the chemical coagulation/precipitation as a
pretreatment can remove phosphorus effectively and can apply MBR-based municipal wastewater treatment.
Keywords: coagulants, correlation, phosphorus removal, pretreatment, zeta potential
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1. Introduction
Phosphorus in wastewater is an important environmental pollutant
with regard to eutrophication (Cooper and Good, 2003; Kiely,
1997), which can in turn disturb the balance of organisms in
water and affect water quality, primarily by depleting the oxygen
supply as algae decay. Reduced oxygen levels have harmful
effects on fish and other aquatic life, causing reductions in
biodiversity. As a consequence, phosphorus removal and recovery
from wastewater are considered important goals of environmental
sustainability (Morse et al., 1998). The Total Phosphorus (TP) in
water routinely is differentiated into three fractions based on
common analytical measurements: 1) soluble reactive phosphate,
2) soluble organic phosphorus and particulate phosphorus. The
Soluble and particulate phosphorus are differentiated by whether
or not they pass through a 0.45 µm-pore glass fiber (Spivakov et
al., 1999).
The removal of phosphorous from wastewater involves the
incorporation of phosphate into Total Suspended Solids (TSS)
and the subsequent removal of these solids. Phosphorous can be
incorporated into biological solids (e.g., microorganisms) or
chemical precipitates. Chemical phosphorus removal entails the
removal of inorganic phosphate forms through the addition of a
coagulant and the mixing of wastewater and coagulant. The
multivalent metal ions that are most commonly used as coagulants
are calcium, aluminum, and iron (US EPA, 1976; Sawyer et al.,
1994; Morse et al., 1998; Jiang and Graham, 1998; Spivakov et
al., 1999). In biological phosphorus removal, an anaerobic tank
(in which nitrate and oxygen are absent) is placed upstream of
the aeration tank. Under these conditions, a group of heterotrophic
bacteria, called Polyphosphate-Accumulating Organisms (PAOs),
selectively enrich in the bacterial community of the activated sludge.
These bacteria accumulate large quantities of polyphosphate, and
this biomass is separated from the treated water at the end of the
process-phosphorus is thus removed (Thomas et al., 1996; Clark
et al., 1997; de Hass et al., 2000; Henze et al., 2002; Ebeling et
al., 2004; Tykesson et al., 2005).
Since the biological phosphorus removal has shown a relatively
high level of instability due to the competition between PAOs
and Glycogen Accumulating Organisms (GAOs), the sequential
chemical treatment after biological treatment is required to
satisfy strict water quality requirements (0.5 mg/L as P) (Johnson
et al., 2006; Willson and McGettigan, 2007; US EPA, 2009).
Chemical pretreatment prior to biological treatment is not a
routine process but can improve the removal efficiencies of
suspended organics and TP over conventional primary settling
(Gujer and Boller, 1978). An advantage of chemical coagulation
as a pretreatment is that it potentiates the development of a
compact primary settling tank and secondary biological treatment
system because coagulants improve settleability by enhancing

*Member, Professor, Dept. of Civil and Environmental Engineering, Hanyang University, Seoul 133-791, Korea (E-mail: jk120@hanayng.ac.kr)
**Member, Principal Researcher, R&D Center, Samsung Engineering Co. Ltd., Suwon 443-823, Korea (Corresponding Author, E-mail: jin-wook.chung@
samsung.com)

− 956 −
 Implementing Chemical Phosphorus Removal as Pretreatment
flocculation and remove inhibitory compounds, such as pesticides
and heavy metals (Levine et al., 1985; Reynolds and Richards,
2000; Saeparastzadeh et al., 2007). Also, in Membrane Bioreactor
(MBR), fouling precursors, such as Suspended Solids (SS) and
colloidal particles in raw wastewater, coagulate and flocculate
due to the addition of chemicals, thereby decreasing the occurrence
of fouling (Bacchin et al., 1995; Harmant and Aimar, 1996;
1998; Kim et al., 2011).
Chemical coagulation is the most important step in removing
colloidal particles and turbidity from wastewater, causing
contaminants, ranging from 0.1 µm to 10 µm, to aggregate
(Bacchin et al., 1995); yet, easily biodegradable organic compounds,
as well as colloidal particles and phosphorus, are removed in this
step undesirably. This phenomenon results in the excessive
addition of coagulants and expensive operation costs. In general,
several factors affect chemical phosphorus removal: 1) the
composition of phosphorus species in raw wastewater; 2) the
molar ratio of metal to influent phosphorus concentration (Al to
P or Fe to P); 3) the choice and dose of coagulants; 4) the
location and number of feed points; 5) the pH; and 6) the mixing
(dispersion) conditions (Ahn and Park, 2008; Bliss et al., 1994;
de Haas et al., 2001; Ahmed et al., 2005; Caravelli et al., 2010;
Zhang et al., 2010).
The objectives of this study were to investigate the factors that
affect chemical phosphorus removal as a pretreatment for
municipal wastewater. We examined various doses of 2 coagulants
(PAC and ferric chloride), pH, and mixing conditions for 5 types
of municipal wastewater. The relationship between TP removal
and SS, Total Organic Carbon (TOC), Total Nitrogen (TN),
turbidity, and color removal was determined. We investigated
coagulation efficiencies depending on the presence of particulate
phosphorus using raw wastewater and filtered wastewater. Finally,
we evaluated whether chemical coagulation/sedimentation can be
applied as a pretreatment and determined the optimal design and
operational factors for its use for municipal wastewater.
2. Materials and Methods
2.1 Experimental Setup and Conditions
Raw municipal wastewater was obtained from 5 municipal
wastewater treatment plants in Kyoto, Japan. All wastewater,
used as experimental feed in this study, was taken before a
primary clarifier.
In order to investigate the effect of selection and dose of
coagulants, coagulation experiments were performed at room
temperature in a 6-paddle stirrer apparatus (Miyamoto Co.,
LTD.) in 2-L jars using the following conditions: mixing at 100
rpm for 2 min, addition of coagulant, mixing at 100 rpm for 5
min (rapid mixing) and at 30 rpm for 10 min (slow mixing),
settling for 30 min, and decantation. The reaction mixture was
stirred at room temperature and pH in wastewater was
unadjusted. The velocity gradient (G) was set to 92.2 (1/sec) for
the rapid mixing and shifted to 15.2 (1/sec) for the slow mixing.
Vol. 18, No. 4 / May 2014 − 957 −
Table 1. Experimental Conditions of GT Value
Rapid mixing Mixing Slow mixing Mixing
GT
Run No. (G value : time (G value : time
values
1/sec) (min) 1/sec) (min)
1 92.2 1.5 15.2 5 12,780
2 92.2 2 15.2 7 17,340
3 92.2 3 15.2 10 25,560
4 169.6 3 42.8 10 56,400
5 169.6 6 42.8 20 112,800
Others: 5 min settling and then 100 (mL) sampling from the water sur-
face for analysis.
PAC (30.5% w/ v) and ferric chloride (60% w/w) as coagulants
were purchased from Chemland Co. (USA) and Spectrum
Laboratory Products Inc. (USA), respectively. The coagulation
test was conducted using 2 feed types-unfiltered wastewater and
wastewater that was filtered through a 0.45 µm-pore glass fiber
filter to verify the characteristics of coagulation depending on the
composition of TP.
In determining the effect of pH on coagulation, the pH was
adjusted to the desired level (ranged from 4 to 9) with 0.2 N HCl
or 0.2 N NaOH. Ferric chloride as coagulant and raw wastewater
collected from plant K was used. All other experimental
condition was same as the previous coagulation experiment. To
test the mixing effect, GT values depending on mixing velocity
and time were varied from 12,780 to 112,800. The detail
experimental conditions for mixing are described in Table 1. In
this experiment, both coagulants and raw wastewater obtained
from plant R were used. Finally, to evaluate the zeta potentials as
an indicator of coagulation, raw wastewater and filtered
wastewater obtained from plant R were added different dose of
coagulants. The mixing velocity and time were same as the
previous coagulation experiment.
2.2 Analysis
The following items were measured in our water quality
analysis of the samples: alkalinity, pH, SS, TOC, TN, TP, zeta
potential, turbidity, color, and metal ions. Alkalinity was determined
as Ca(OH)2 by titration with hydrochloric acid in aqueous
solution. TOC was analyzed with a TOC analyzer (TOC-5000,
Shimadzu, Japan). Zeta potential was measured on a zeta
potential analyzer (ZEECOM, MICRO TECH Co., LTD). Turbidity
and color were measured with a turbidity/color meter (TC-301,
CKC Co., LTD). Metal ion concentrations were analyzed by
inductively coupled plasma-atomic emission spectrometry (ICP-
AES) (ICPS 4960, Shimadzu, Japan). Particle size distribution
analysis was also done using laser diffraction spectroscopy
(Beckman Coulter LS230).
The remaining analyses for pH, SS, TN, and TP were conducted
using standard methods (APHA et al., 1998). All experiments
and measurements were performed in duplicate, and the results
of the water quality analysis were expressed as the mean value of
2 identical samples.
 Jong-Oh Kim and Jinwook Chung

Table 2. Water Qualities of Municipal Wastewater at Five Municipal Wastewater Treatment Plants
Item Alkalinity TOC T-P T-N Zeta-potential Turbidity Color
SS (mg/L) (mg/L) (mg/L) (mV) (NTU) (mg/L)
pH (mg/L as
(mg/L)
Plant CaCO3) W/O filt. Filt W/O filt. Filt. W/O filt. Filt. W/O filt. Filt. W/O filt. Filt. W/O filt. Filt.
K 6.91 110 120 64 44 4.3 2.5 47 37 - - 50.2 17 168.8 82.3
T 6.54 104 98 68 32 7.3 3.1 27 21 - - 38.1 0.8 163.3 90.9
F 6.51 92.3 113 71 37 6.4 2.7 31 25 - - 51.7 2.7 358.0 134
I 6.49 94.1 103 53 26 5.5 2.5 29 23 - - 38.1 0.2 165.3 91.0
R 6.80 146 123 83 32 8.1 4.7 34 19 -22.3 -25.4 58.5 8.9 395.2 106

Item Al Fe Cr Cu Ni Cd Zn Pb Mn K Mg Ca
Plant (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L) (mg/L)
K 0.9(0.2) 0.6(0.2) 0(0) 0(0) 0.1(0) 0(0) 0.1(0.1) 0(0) 0.1(0) 5.5(5.1) 6.8(5.9) 24.8(22.6)
T 1.0(0.3) 0.7(0.3) 0(0) 0(0) 0.1(0) 0(0) 0.1(0.1) 0(0) 0.1(0.1) 4.2(3.1) 5.5(3.9) 12.1(9.6)
F 1.3(0.5) 1.4(0.7) 0(0) 0(0) 0(0) 0(0) 0(0) 0(0) 0.1(0.1) 1.1(0.9) 2.2(2.0) 05.2(4.2)
I 0.9(0.3) 0.8(0.3) 0(0) 0(0) 0(0) 0(0) 0(0) 0(0) 0.1(0) 0.6(0.4) 3.7(2.8) 07.1(5.3)
R 0.4(0.1) 1.5(0.5) 0(0) 0(0) 0(0) 0(0) 0(0) 0(0) 0(0) 1.5(1.1) 8.8(7.9) 16.4(15.2)
*The value in parentheses means the concentration of municipal wastewater after filtration.

3. Results and Discussion

3.1 Characteristics of Municipal Wastewater

To compare the optimal values for the selection and dose of the
inorganic coagulant for coagulation in existing municipal wastewater
treatment plants, we examined the water quality of samples of
municipal wastewater. Table 2 shows that the water quality
differed little between the 5 municipal treatment plants.

3.2 Effect of Selection and Dose of PAC and Ferric Chlo-

ride on Coagulation
The relationship between coagulant dose and removal ratio in
the wastewater from 5 municipal treatment plants is shown in
Fig. 1. The removal efficiencies of SS, TOC, TP, and TN are
described as a function of PAC and ferric chloride dose.
As shown in Fig. 1, more than 50% of the SS and TP were
removed at all doses of PAC and ferric chloride. Although the
efficiencies of SS and TP removal rose with increases in
coagulant dose, those of TOC and TN increased little. When the
removal efficiency for SS peaked, that of TP did as well at the
same coagulant dose. For most contaminants, such as TOC, TN,
TP, and SS, PAC effected higher efficiencies than ferric chloride
in the 5 municipal wastewater samples.

3.3 Coagulant-dependent Relationship between TP

Removal and Other Water Qualities
The relationship between TP removal and other water quality
parameters is shown in Fig. 2. TP removal and SS removal
correlated significantly, whereas TP removal and Total Nitrogen
(TN) removal did not form any discernible relationship. The Fig. 1. Relationship between Coagulant Dose and Removal Ratio
reason is that the dissolved nitrogen was difficult to coagulate for Fresh Sewage (Initial pH for Plant K, T, F, I and R were
with chemical coagulants such as PAC and ferric chloride based 6.9, 6.5, 6.5, 6.5 and 6.8, Respectively)
on the high ratio of total dissolved nitrogen to TN (see Table 2).
In contrast, TP and SS in wastewater could be removed and dissolved phosphorus.
simultaneously, because chemical coagulants can remove particulate PAC had modestly better effects than ferric chloride on

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 Implementing Chemical Phosphorus Removal as Pretreatment

turbidity removal. Ferric chloride precipitated robustly in the

form of ferric hydroxide, with a charge near zero; it is an
extremely hygroscopic species and thus dramatically increases
the volume of the sludge that is generated (Dzombak and Morel,
1990; Delgado et al., 2003).
The coagulant doses that were required to achieve 90% TP
removal were calculated based on the relationship between
coagulant dose and TP removal at each municipal wastewater
plant (Fig. 3). Since a removal rate of TP was achieved over
90%, TP concentration in effluent can be satisfied below 0.5
(mg-P/L) as water quality standards. For raw wastewater, the
required doses of PAC and ferric chloride to attain a 90%
removal rate of TP were 12-20 (mg-Al/L) and 9-18 (mg-Fe/L),
respectively. The average molar ratios of Al to P and Fe to P
were 12.7 and 2.5, respectively. In contrast, for filtered wastewater,
the required doses of PAC and ferric chloride were 10-19 (mg-
Al/L) and 12-24 (mg-Fe/L), respectively. Also, the average molar
ratios of Al to P and Fe to P were 15.6 and 5.3, respectively.
TP removal from raw municipal wastewater by ferric chloride
was more efficient compared with PAC, but PAC removed more
TP than ferric chloride after filtration. The difference in TP

Fig. 2. Correlation between TP Removal and Other Water Quality Fig. 4. Particle Size Distribution for Raw Wastewater and Chemically
Parameters Treated Water

Fig. 3. Required Coagulant Doses for 90% TP Removal (unit: mg/L): (a) Raw Wastewater, (b) Filtered Wastewater

Vol. 18, No. 4 / May 2014 − 959 −

 Jong-Oh Kim and Jinwook Chung

removal efficiencies can be attributed to the size distribution of
particles in wastewater, whereby PAC is effective when most of
the particles in wastewater are below 1 µm, whereas ferric
chloride might predominate when the particles are over 1 µm
(Fig. 4).
The hydrophobic:hydrophilic material ratio in municipal
wastewater also might have influenced these results. Nevertheless,
selecting the optimal coagulant for a treatment facility depends
on many other factors in addition to those that we have
discussed.
3.4 Effect of pH on TP, TOC, Turbidity and Color Removal
pH regulates coagulation, and the efficiency of coagulation of
settled tannery wastewater depends on the control of pH and the
coagulant dose (Song et al., 2004). Therefore, we measured the
effects of pH on TOC, turbidity, color, and TP removal between
pH 4.0-9.0 (Fig. 5).
The optimal pH for TOC removal was approximately 6.0, and
the overall removal efficiencies were slightly lower than those
for turbidity, color, and TP removal. Turbidity and color removal
rates at pH 6.5 were approximately 94% and 86%, respectively,
at 12 mg-Fe/L. Although the optimal pHs for the highest
removal rate of TOC, turbidity, color and TP were somewhat
different, the same pattern of removal for all contaminants were
observed.
The highest TP removal efficiency was observed at pH 6.5
and a ferric chloride dose of 12 mg-Fe/L (molar ratio of Fe to
P was 5.7). As the pH fell below the neutral range (6.0-7.0),
TP removal efficiencies decreased dramatically. Theoretically,
ferric chloride decreased effluent phosphorus concentrations
to 0.01 mg/L between pH 6.6 and 7.2 (WEF and ASCE,
1998).
The optimal pH range in this study was slightly narrower than
previous results. Smith et al. (2007) reported that the highest
phosphorus removal efficiency occurred between pH 5.5 and
7.0. Because PAC and ferric chloride are acidic and, therefore,
capable of lowering pH, adjustments to the pH might be needed
to achieve high removal efficiencies when the alkalinity is
insufficient to buffer the wastewater adequately.
The optimal pH range will be site-dependent, due to other
chemical reactions that occur in the wastewater. Also, to remove
phosphorus completely, the exact coagulant dose with regard to
pH must be estimated, which can be difficult (Johnson and
Amirtharajah, 1983; US EPA, 2008).
3.5 Effect of Mixing on Coagulation
Rapid mixing is required to allow molecules to react when a
chemical is added to wastewater. In addition, the density and
viscosity of metal salts are larger than those of wastewater, which
allows the chemical to settle.

Fig. 5. pH versus Removal Efficiency at Various Doses (Conditions; TOC 83 mg/L, Turbidity 58.5 NTU, Color 168.8 mg/L, Coagulant: Ferric
Chloride, Raw Wastewater was Obtained from Plant K): (a) TOC Removal, (b) Turbidity Removal, (c) Color Removal, (d) TP Removal

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 Implementing Chemical Phosphorus Removal as Pretreatment
Fig. 6. Relationship between GT and Removal Ratio (Conditions:
TOC 110 mg/L, pH 6.8, Dose: Ferric Chloride 6 mg/L, Tem-
perature: 20oC, Raw Wastewater was Obtained from Plant R)
Figure 6 shows the effect of mixing (GT value) on coagulation.
The favorable range of GT values for wastewater coagulation is
23,000-210,000 (Tchobanoglous et al., 2004). In our experiment,
although SS removal rose slightly with increases in GT value,
there was no significant difference in the removal of TOC,
turbidity, and color between GT values of 12,780 and 112,800,
because the extent of mixing between the flocculating agent and
particles was sufficient in this experiment.
3.6 Zeta Potential as an Indicator of Coagulation
The adsorption-destabilization of colloids (particles) indicates
that coagulation occurs when repulsive electrical forces between
particles are at a minimum. One measure of particle charge is the
zeta potential. It is possible to determine the zeta potential of
particles in a particular system from the velocity at which these
particles traverse a measured path in a DC current at a specific
voltage; this velocity is the electrophoretic mobility.
Fig. 7. Zeta Potential versus Inorganic Coagulant Doses (Conditions: pH 6.6-6.8, TOC 95-120 mg/L, Temperature: 20oC, Raw Wastewater
was Obtained from Plant R): (a) Raw wastewater, (b) Filtered wastewater
Vol. 18, No. 4 / May 2014 − 961 −
In practice, optimal coagulation occurs at electromotive force
or zeta potential values that are less than or greater than zero
(Johnson and Amirtharajah, 1983). Generally, a suspension is
stable if the magnitude of the average zeta potential exceeds 20
mV (|ζ| > 20 mV), whereas rapid coagulation occurs if the
particles have zeta potentials between -10 mV and 10 mV. The
critical coagulant concentration is generally defined as the
coagulant dose that is required to revert the average particle zeta
potential to 0 ± 1 mV. The critical coagulant dose also depends on
mixing rates and initial solution composition (pH, ionic strength,
alkalinity, and TOC concentration) (Edward et al., 1991).
Figure 7 shows the variation in zeta potential with increases in
coagulant dose. The average particle zeta potential for raw
wastewater and filtered wastewater before the addition of
coagulant were 7.3 and 5.5 mV, respectively. Particle zeta
potentials increased steadily (became less negative) with rises in
the dose of both coagulants. Previously, expected coagulant
doses were estimated using the TP removal rate as a parameter of
evaluation. The zeta potential was approximately -2.2 to -0.7
(mV) between 8~16 (mg/L) ferric chloride; for PAC, the zeta
potential ranged between -9.6 to -0.6 (mV) at the same coagulant
dose for raw wastewater.
In raw water, the zeta potential of ferric chloride solution was
higher (or less negatively charged) than that of PAC, whereas
this pattern was reversed in filtered wastewater. This result
implies that the fraction of colloidal materials in filtered
wastewater is relatively higher than that in raw wastewater,
based on previous findings that PAC is more effective in
removing colloidal materials than ferric chloride when same
dose of coagulant was added (Hlavacek and Remy, 1995).
Both the required coagulant dose in zeta potential ranges that
are favorable for coagulation and the estimated necessary
coagulant dose for a TP removal rate of 90% had similar ranges
under similar pH condition (6.6-6.8). Based on these results, we
believe that the zeta potential is an adequate parameter for
defining appropriate coagulant doses.
 Jong-Oh Kim and Jinwook Chung
4. Conclusions
The factors that affect chemical phosphorus removal as a
pretreatment for MBR-based municipal wastewater treatment
were investigated with regard to the dose of 2 coagulants (PAC
and ferric chloride), pH, and mixing conditions. Based on our
experimental results, the correlation between TP removal and
other water quality indicators was evaluated. PAC effected higher
efficiencies than ferric chloride for 5 municipal wastewater
samples. TP removal and SS removal correlated significantly,
although TP removal and TN removal did not. PAC was slight
more effective than ferric chloride with regard to turbidity and
color removal. Also, at the same dose of coagulant, TP removal
from raw wastewater by ferric chloride was greater than with
PAC, but PAC was superior to ferric chloride when filtered
municipal wastewater was treated. The dose of coagulant and the
removal of phosphorus were highly sensitive to pH, but the
removal of TOC, turbidity, and color did not differ between GT
values of 12,780 and 112,800. The chemical coagulation/
precipitation as a pretreatment can remove phosphorus effectively
and can apply MBR-based municipal wastewater treatment.
Acknowledgements
This study was supported by the National Research Foundation
of Korea (NRF) grant funded by the Korea government (NRF-
2013R1A2A1A09007252).
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