Journal of Environmental Management 206 (2018) 1126e1134

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Journal of Environmental Management

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Research article

Operating cost reduction of UF membrane filtration process for

drinking water treatment attributed to chemical cleaning
optimization
Sung Soo Yoo a, Kyoung Hoon Chu b, Il-Hwan Choi c, Ji Sung Mang a, Kwang Baik Ko a, *
a
Department of Civil and Environmental Engineering, Yonsei University, 134 Shinchon-dong, Seodaemun-gu, Seoul, 120-749, South Korea
b
Department of Civil and Environmental Engineering, University of South Carolina, 300 Main St., Columbia, SC, 29208, USA
c
Water Analysis and Research Center, Korea Water Resource Corporation, Shintangin-ro 200, Daeduk-gu, Daejeon, 34350, South Korea

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

Article history: This study investigated the cost and CO2 emission reduced as a result of optimizing operating conditions
Received 18 December 2016 for chemical cleaning in a membrane filtration process used for water treatment. A new protocol was
Received in revised form proposed and operating conditions for chemical cleaning of a pilot-scale membrane filtration process
11 February 2017
were optimized. The critical flux for irreversibility was identified as the permeate flux using a modified
Accepted 26 February 2017
Available online 8 December 2017
flux-step method, and was 100 l m
2 h
1, 20 l m
2 h
1 higher than the vendor recommended permeate
flux. NaOCl, which is also the vendor recommended chemical, was selected as the optimal chemical
reagent following an examination of the permeability restoration ratios and nature of the irreversible
Keywords:
Irreversible fouling
foulants. The optimized operating conditions of enhanced flux maintenance (EFM), determined using
Chemical cleaning optimization response surface methodology (RSM) were: 6.3 d interval, 500 ppm concentration, and 76 min duration,
Operating cost reduction which represented an increase of 4.3 d, 300 ppm, and 36 min, respectively, as opposed to the vendor
Enhanced flux maintenance recommended conditions. As a result, the total operating cost and CO2 emission were $0.1187/m3 and
Response surface methodology 112.75 g CO2/m3, respectively, and 26.5% lesser compared to the operating cost and CO2 emission based
on vendor recommended conditions. This study found that the reductions in operating cost and CO2
emission using the optimization process were excellent.
© 2017 Published by Elsevier Ltd.

1. Introduction chemicals, membrane replacement, energy, and sludge disposal as

In recent years, despite strict effluent quality standards to pro-
vide high-quality drinking water, the quality of drinking water re-
sources has gradually deteriorated due to industrialization and
urbanization. It is becoming increasingly difficult to meet effluent
quality standards with conventional drinking water treatment
processes (Esplugas et al., 2007; Saleem et al., 2016; Zhou and
Smith, 2002) and research on advanced drinking water treatment
processes is underway. Water treatment using membrane filtration
process has received attention due to its advantages such as
excellent effluent quality, easier process management, and smaller
ecological footprint compared to conventional processes
(Kingsbury and Li, 2009; Zhang et al., 2014). However, its drawback
include relatively higher operating costs including costs of labor,
* Corresponding author.
E-mail address: kbko@yonsei.ac.kr (K.B. Ko).
opposed to other processes (Lopes et al., 2013; Yoon et al., 2004).
During the membrane filtration process, a fouling phenomenon
occurs where organic or inorganic materials accumulate on either
side of the membrane surface or in the membrane pores as oper-
ating time increases (Choi et al., 2008; Fabris et al., 2007). This
reduces flux and increases trans-membrane pressure (TMP) (Nerger
et al., 2015), thereby degrading performance and increasing energy
and membrane replacement costs. Irreversible fouling occurs when
the particles form a matrix strongly attached to the membrane
surface and cannot be removed through physical cleaning methods,
like pore blocking, clogging, biofilm, and cake gel (Kimura et al.,
2004; Lo pez-Roldan et al., 2016; Zularisam et al., 2006). Irrevers-
ible fouling can be removed by chemical cleaning only which is,
therefore, a critical factor that can influence the operating costs of
the membrane filtration process (Blanpain-Avet et al., 2004; Howe
and Clark, 2002; Lodge et al., 2004).
Chemical cleaning of the membrane enables safer operation by
removing irreversible fouling using acids, bases, or oxidants

https://doi.org/10.1016/j.jenvman.2017.02.072
0301-4797/© 2017 Published by Elsevier Ltd.
 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134
(Kuzmenko et al., 2005; Peter-Varbanets et al., 2011), decreasing
the reduction of flux and increasing TMP. However, excessive
chemical cleaning can damage the membrane surface, resulting in
increase in membrane replacement cost, chemical cost, and sludge
disposal cost. In addition, insufficient chemical cleaning cannot
eliminate fouling completely and can lead to additional chemical
costs that eventually increase operating costs (Chen et al., 2003a;
Regula et al., 2014). Therefore, the operating conditions for chem-
ical cleaning need to be optimized to reduce operating costs of the
membrane filtration process.
The operating conditions of chemical cleaning are cleaning
interval, cleaning duration time, chemical type, and chemical
concentration. Energy consumption, chemical use, and sludge
production in the membrane filtration process are reduced by
operating condition optimization, and membrane replacement
cycle is increased by it. This means operating cost reduction in
economical aspects as mentioned above and CO2 reduction in
environmental aspects. Currently, Korea has established green-
house gas(GHG) reduction roadmap in order to reduce GHG
estimation for 2020 business-as-usual by 30% and is enforcing
varous national policies to reduce CO2 emission. Drinking water
and wastewater treatment field also needs to develop and
study new technologies to reduce CO2 (Kim et al., 2011). The
operating condition optimization of chemical cleaning in mem-
brane filtration process is considered to be one of the ways to
satisfy this.
In order to optimize operating condition, it is important to un-
derstand the characteristics of accumulated irreversible fouling, a
very complicated phenomenon where membrane characteristics
(membrane materials, pore size, configuration, hydrophobicity,
charge), process operating conditions (TMP, temperature, permeate
flux), and the physicochemical characteristics of the influent (par-
ticle size distribution, inorganic or organic mattes) closely influence
each other. Hence, it is difficult for general operators to correctly
understand the characteristics of irreversible fouling and deter-
mine appropriate operating conditions (Al-Amoudi and Lovitt,
2007; Gao et al., 2011; Kimura et al., 2004). Additionally, exten-
sive experiments need to be conducted to optimize factors that
affect chemical cleaning itself, such as the chemical interval,
duration, reagent, and concentration (Gernaey et al., 2004). Thus, it
is not practical to perform such experiments at pilot- or full-scale in
terms of cost and time. Therefore, most membrane filtration facil-
ities in operation conduct chemical cleaning using vendor
Fig. 1. Schematic diagram of pilot-scale plant used in this study.
1127
recommended conditions that are not the optimized operating
conditions.
Most of the previous studies conducted on the optimization of
chemical cleaning have aimed to increase the efficiency of fouling
removal (Bogati et al., 2015; Kim et al., 2011; Strugholtz et al., 2005;
Zondervan et al., 2008). Although a few studies focused on cost
reduction of the membrane filtration process, it was difficult to
apply the protocols in practice, as they were very complicated, or
were likely to cause errors when they were applied to a pilot- or
full-scale plants because they were carried out as lab-scale exper-
iments (Porcelli and Judd, 2010b). The objective of this study was to
investigate the reduction of operating cost and CO2 emission that is
achieved by optimizing the operating factors for chemical cleaning
of the membrane. A new protocol was proposed to optimize the
operating conditions and the operating conditions for chemical
cleaning of a pilot-scale membrane filtration process were opti-
mized based on the protocol proposed. In addition, the pilot plant
was operated for 2 months under the optimized operating condi-
tions to investigate the costs saved.
2. Materials and methods
2.1. Experimental setup
This study was conducted using a pressurized UF membrane
filtration process for drinking water treatment in a pilot-scale plant
installed in an existing drinking water treatment facility. The
schematic diagram of the pilot-scale plant is illustrated in Fig. 1. A
pressurized UF membrane developed by Cheil industry, made of
PVDF, pore size 0.01 mm, surface area 72 m2 and length 2.16 m, was
used as the membrane module. Raw water was collected from the
front part of sand filtration unit in the water treatment facility, and
three samples a week were collected for analysis. The pH and
conductivity of raw water was determined using DWA-2000A and
YSI-30, respectively, and its turbidity was analyzed using HACH
SC200. GE 5310C was used for the analysis of TOC and DOC, and
HACH DR4000 was used for UV254. Inorganic materials, such as Fe
and Mn, were analyzed using the standard 3120D digestion method
employing ICP-AES. The characteristics of raw water used are pre-
sented in Table 1. Operating mode was cross-flow with permeate
time of 29 min and backwash time of 1 min. Permeate flux was
80 l m
2 h
1, backwash flux was 120 l m
2 h
1, and the air flow of
air scrubbing during backwash was 0.3 Nm3 h
1 m
2.
2.2. Chemical cleaning method
The chemical cleaning methods commonly used in the industry
are clean-in-place (CIP), chemical enhanced backwash (CEB), and
enhanced flux maintenance (EFM) (Hu et al., 2013; Lin et al., 2010;
Porcelli and Judd, 2010a). CIP and EFM were used as chemical
cleaning methods for the membrane filtration process in this study.
CIP was conducted when permeability dropped to 70% of the initial
permeability level, using 1000 ppm of sodium hypochlorite (NaOCl)
and citric acid (pH 2.0) for 12 h. EFM, like CEB, is a chemical
cleaning method that extends the cycle of CIP. CEB is a method that
uses chemicals to perform backwash, while EFM is a method where
soaking is performed with a chemical for a certain duration at a
certain interval. The generally recommended chemicals for EFM
include NaOCl, sodium hydroxide (NaOH), citric acid, and hydrogen
chloride (HCl) with 1e7 d interval, 100e500 ppm concentration,
and 10e90 min duration. Vendor recommended operating condi-
tions that were used in the plant in this study were: 200 ppm of
NaOCl, 2 days of chemical interval, and 40 min of duration time. In
this study, the operating conditions of the EFM in the pilot plant
were optimized.
1128 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134

Table 1
Concentrations of influent raw water.

Constituents (unit) Average Range

pH (median) 7.55 7.0e8.9

Turbidity (NTU) 2.54 1.3e4.8
TOC (mg/L) 1.29 1.08e1.45
DOC (mg/L) 1.02 0.91e1.21
Total Fe (mg/L) 0.11 0.09e0.12
Total Mn (mg/L) 0.05 0.045e0.054
Total Al (mg/L) NDa e
Cl2 (mg/L) 0.25 0.07e0.51
Conductivity (mS/cm) 249 201e412
Ionic strength (mol/L) 0.003 0.003e0.005
Temperature ( C) 19.3 18e22
UV254 (cm
1) 0.04 0.032e0.055
a
ND: not detected.

2.3. New protocol for operating condition optimization

The protocol developed for optimization of chemical cleaning

consisted of three steps. The characteristic of the protocol proposed
newly is to consider permeate flux as one of the operating condi-
tions of chemical cleaning and determine optimum operating
conditions as minimum experiment by statistical analysis in order
to improve field applicability. The flowchart of the protocol is
shown in Fig. 2.
Permeate flux and chemical reagent were identified prior to
optimization of other operating conditions such as chemical in-
terval, duration, and concentration as the permeate flux influences
the quantity of fouling accumulated on the membrane surface, thus
affecting the chemical interval. The optimal chemical reagent was
also determined prior to optimization of chemical concentration
and duration, as the substances that can be removed differ with
each chemical reagent. Subsequently, the optimal permeate flux
was determined in step 1. Then, the optimal chemical reagent was
decided based on an investigation of the permeability restoration
and major foulants in step 2. Finally, response surface methodology
(RSM), a statistical method, was used to determine optimal con-
ditions using minimum experiments.

2.3.1. Permeate flux determination

A modified flux-step method proposed by previous research Fig. 2. Flow-chart of newly developed protocol e description of the three-step process
was used to determine the permeate flux (Chu et al., 2014). The undertaken to optimize operating conditions for chemical cleaning.
modified flux step method included physical cleaning methods
such as backwash, membrane tank drainage and relaxation in the
flux-stepping tests. The threshold flux and critical flux for irre- where, p is the TMP, n is the flux-steps; t is the flux-step duration
versibility were determined using the data obtained. The flux- (h), b is the backwashing duration (h).
stepping test was performed three times from 20 l m
2 h
1 to
160 l m
2 h
1 with the step height of 20 l m
2 h
1. The step  Total membrane resistance:
duration was 29 min and the backwash duration was 1 min. The
DP
backwash flux was 1.5 times filtration flux, and the membrane tank Rtot ¼ Rm þ Rads þ Rrev þ Rirrev ¼ (3)
mJ
was drained every time the flux-step was increased or decreased.
TMP and flux data obtained through the flux-stepping test were
where, m is viscosity (Pas), J is permeate water flux (m/s), Rtot is the
used to calculate the fouling rate and membrane resistance as
total filtration resistances including clean membrane Rm, adsorp-
shown in Eq. (1), Eq. (2), and Eq. (3)).
tion Rads, reversible fouling Rrev, and irreversible fouling Rirrev
(1011m
1) (Field and Pearce, 2011).
 Total fouling rate:
n
Pn
Pend
Ftot ¼ initial
(1) 2.3.2. Chemical reagent determination
Dt In order to choose an optimal chemical reagent, the restoration
ratio of permeability and irreversible foulant were examined. The
 Irreversible fouling rate: permeability of the fouled membrane before and after chemical
cleaning, J0 and J1, respectively, were measured to calculate the
n2 n1 permeability restoration ratio. An acid (citric acid, pH 2.0), a base
Pinitial
Pinitial
Firrev ¼ (2) (NaOH, pH 12.0), and an oxidant (NaOCl, 500 ppm) were used as
Dt þ Db
chemicals. To accumulate irreversible fouling within a short-term,
 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134
only one backwash was performed per week, without chemical
cleaning, and the permeate flux used was 140 l m
2 h
1 that is
higher than the critical flux for irreversibility determined in step 1.
To investigate irreversible foulant, fluorescence excita-
tioneemission matrices (FEEM) (Tecan Xflour4 Safire II, Germany),
and Fourier-transform infra-red (FTIR) (Vertex 70, Bruker, MA, USA)
analyses were performed.
2.3.3. Operating condition optimization
RSM was performed in the order of experimental design,
response surface design analysis, and response surface analysis
optimization. A central composite design (CCD) was used to design
experiments randomly. After the experiment was designed,
response surface design analysis was carried out on the results and
quadratic regression models with an independent variable k were
determined, as shown in Eq. (4).
X
k X
k X
k
Y ¼ b0 þ bi $xi þ bii $ x2i þ bij $xi $xj þ ε
i¼1 i¼1 ij
where, Y is the response variable, xi and xj are the ith and jth coded
independent variables, respectively.
To test the validity of the determined regression models, t-test,
analysis of variance (ANOVA), lack-of-fit test, residual analysis, and
calculation of root mean square error (RMSE) for experiment data
and predicted data were conducted. The calculation of RMSE was
based on Eq. (5) below.
sffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
Pn 2
i¼1 ðXi
Yi Þ
RMSE ¼
n
1
where, Y is the response variable; xi and xj are the ith and jth coded
independent variables, respectively, Xi is the experimental data, Yi
is predicted data by regression models and n is the number of ex-
periments performed.
As the number of response variables to be optimized was one or
more, multiple response surface methodology (MRSM) was used
(Ahn et al., 2014; Myers et al., 2009). The desirability function,
which is an efficient method of to standardize the result values
with different units by converting the results into values between
0 and 1, was used. The desirability value of 1 means an access with
great satisfaction to the target to be sought for, while 0 means that
the result was obtained below a criterion. Overall desirability is
defined by the geometric mean of respective desirability, which is
available as a rating scale of the MRSM optimization (Li et al., 2007).
2.4. Calculation of operating cost and CO2 emission
Operating costs with the vendor recommended conditions were
compared with those of optimized conditions. The pilot-scale plant
used in this paper was operated for two months under the opti-
mized conditions. Operating costs, energy (power) cost, chemical
cost, and sludge disposal cost were calculated, while the common
costs such as labor and membrane replacement were not
considered.
The CO2 emissions reduction by chemical cleaning optimization
of membrane filtration process were calculated through the Global
Warming Potential (GWP) category of life cycle assessment (LCA).
The LCA analysis was carried out using a TOTAL program, a
modeling program developed by Korea Environmental Industry
and Technology Institute. As a life cycle inventory (LCI) database, a
national LCI database developed by the ministry of environment
and the ministry of knowledge and economy, and provided by the
korea environmental industry and technology Institute, was used.
1129
For the chemical reagent which was not included in the national LCI
database, an ecoinvent database developed by Switzerland was
used. The parameter and sources of the LCI database used was
shown in Table 2.
3. Results and discussion
3.1. Determination of critical flux for irreversibility (step 1)
Permeate flux can be divided into critical flux, threshold flux,
critical flux for irreversibility, and limiting flux (Field et al., 1995;
Luo et al., 2012). The critical flux for irreversibility represents the
transition between reversible and irreversible fouling (Chu et al.,
2014). In other words, as irreversible fouling is formed only above
the critical flux for irreversibility, and not below, operating at the
critical flux for irreversibility can result in minimizing the interval
of chemical cleaning and maximizing treatment of water. There-
(4)
fore, the critical flux for irreversibility was determined as the most
efficient permeate flux for saving operating costs.
The fouling rate and membrane resistances were calculated
with the flux and TMP data obtained using the modified flux-step
method. The results are presented in Fig. 3.
When the permeate flux was between 20 l m
2 h
1 and
80 l m
2 h
1, Ftot and Firrev were nearly constant at 0.51 kPa h
1 and
0.15 kPa h
1, respectively. The Ftot rapidly increased to 3.58 kPa h
1
at 100 l m
2 h
1, beyond which, Ftot increased with the permeate
flux, reaching 20.25 kPa h
1 at 160 l m
2 h
1. Firrev remained con-
stant at 0.15 kPa h
1 when the permeate flux was increased to
100 l m
2 h
1. However, when the permeate flux was increased to
(5)
120 l m
2 h
1, Firrev rapidly increased to 0.63 kPa h
1, a phenom-
enon called TMP-jumping, and kept constantly increasing to a
maximum level of 3.61 kPa h
1.
In order to select the critical flux for irreversibility, both fouling
rate and membrane resistance were calculated. Membrane resis-
tance was calculated using Eq. (3) and the result is shown in Fig. 4.
In this study, the resistance of clean membrane (Rm) was
4.80  1011 m
1. The resistance caused by surface or pore adsorp-
tion regardless of the flux (Rads) was 0.42  1011 m
1. The resistance
caused by the reversible component (Rrev) when the permeate flux
was 20e80 l m
2 h
1 occurred at insignificant levels and was
ignored; the resistance caused by the irreversible component (Rir-
11
1
at 100 l m
2 h
1 resulting in the
rev) was 0. Rrev was 0.3  10 m

2
1
increase of Rtot. Even at100 l m h , Rirrev barely increased. Rirrev
started to increase at 120 l m
2 h
1 and kept increasing till
160 l m
2 h
1.
The critical flux for irreversibility that minimizes the
frequency of chemical cleaning with the most efficient
operating cost was 100 l m
2 h
1. The reason is that the irre-
versible fouling rate started increasing rapidly at 100 l m
2 h
1.
In addition, the vendor recommended permeate flux of was
80 l m
2 h
1 was determined to be the threshold flux. The dif-
ference in operating costs created by increasing the permeate
flux from 80 l m
2 h
1 to 100 l m
2 h
1 is discussed in detail in
section 3.4.
Table 2
LCI database source used in this study.
Parameter Source
Electricity Korea LCI databasea
Sludge disposal
Chemical reagent (NaOCl) Ecoinventb
a
www.epd.or.kr.
b
www.ecoinvent.org.
1130 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134
Fig. 3. Variation of fouling rate with flux - Change in total membrane fouling rate (Ftot)
and irreversible fouling rate (Firrev) with increase in flux, assessed using modified flux-
step method.
3.2. Determination of optimal chemical reagents
For selecting an optimal chemical reagent, pure water perme-
ability before chemical cleaning (J0) and after chemical cleaning
(J1) were measured, and restoration ratios (J1/J0) were calculated
based on the results. Three types of chemical reagents: an acid
(citric acid), a base (NaOH) and an oxidant (NaOCl) were used. The
analysis results of permeability restoration ratios are shown in
Fig. 5.
J0 was 191.69 l m
2 h
1 bar
1 on an average, and J1 after
chemical cleaning using citric acid, NaOH, and NaOCl was
220.44 l m
2 h
1 bar
1, 299.04 l m
2 h
1 bar
1 and
314.37 l m
2 h
1 bar
1, respectively. NaOCl and NaOH showed the
high restoration ratios (1.64 and 1.58 respectively), and citric acid
showed a low restoration ratio (1.15). Previous studies conducted
on chemical cleaning of membrane filtration process indicated that
NaOCl and NaOH were effective in removing organic matter, and
citric acid was effective in removing inorganic matter. Therefore, it
is assumed that the major foulants were organic matter.
Fig. 4. Variation of resistance with flux rate e Bar graph displays changes in total
resistance, reversible resistance, and irreversible resistance with increase in permeate
flux rate.
Fig. 5. Effect of various chemical reagents on restoration ratios: Bar graph shows ef-
fects of cleaning using citric acid, NaOH and NaOCl on removal of irreversible fouling;
where J0 is pure water permeability before chemical cleaning, and J1is pure water
permeability after chemical cleaning.
However, choosing an optimal chemical reagent between NaoCl
and NaOH was difficult as there was no striking difference in their
permeability restoration ratios. Moreover, though both NaOCl and
NaOH remove organic matter, the kind of organic matter removed
may differ as NaOCl acts as an oxidant and NaOH acts as a base.
Previous studies have indicated that the kind and property of
organic matter forming irreversible foulants determines the effi-
ciency of removal of the organic matter by NaOCl and NaOH
(Kimura et al., 2004).
Therefore, an analysis of the types and characteristics of
organic matter that formed irreversible fouling on the membrane
is required to choose an optimal chemical reagent. FEEM and FTIR
were conducted and results are shown in Figs. 6 and 7,
respectively.
Fig. 6(a) indicates that organic matter removed by NaOCl were
probably humic acid- and fulvic acid-like matter (Chen et al.,
2003b). Therefore, NaOCl can be used for specialized removal of
humic acid and fulvic acid-like matter. Unlike NaOCl, the analysis
result of NaOH (Fig. 6(b)) indicates there were fulvic acid-like
organic matter (Chen et al., 2003b). Therefore, NaOH can be used
to remove various kinds of organic matter including fulvic acid-like
organic matter.
Fig. 7 indicated that both NaOCl and NaOH wash water
showed similar analysis results. Peaks observed typically refer to
organic matter with alkene-based (sp2 carbon double bond),
primary functional groups and the aromatic ring functional
group (sp2 carbon double bond) which include humic acid-like
organic matter (Zularisam et al., 2006). Thus, humic acid-based
organic matter primarily created irreversible fouling, and these
results explain why the permeability recovery rate of NaOCl was
higher than that of NaOH. Finally, NaOCl, an oxidant-based
organic matter cleaning agent specialized in humic acid-like
organic matter cleaning was chosen as the optimal chemical
reagent.
3.3. Operating conditions optimization by RSM
RSM analysis was used to optimize the operating conditions of
EFM. Removal efficiency of irreversible fouling decreased when
only operating cost was considered as a response variable during
optimization of operating conditions. To solve this problem,
 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134 1131

YTMP ¼ 1:69298X1
2:91228X2
1:04386X3 þ 0:1874X12

þ 0:845295X22 þ 1:15231X32
0:4057X1 X2

0:25219X1 X3
0:58114X2 X3 þ 3:64434
(6)

h
YCost ¼
10:517X1 þ 2:503X2 þ 0:53X3 þ 7:097X12 þ 0:004X22

þ 0:007X32
2:11X1 X2
0:352X1 X3 þ 0:072X2 X3

i
þ 123:919  10
3
(7)

Where, X1, X2, and X3 are chemical interval, duration time, and
chemical concentration, respectively.
Statistical significance tests were conducted to consider the
applicability of the regression models. ANOVA, t-test, lack-of-fit
test, residual analysis, and comparison between experimental
data and predicted data were conducted. As result of t-test and
ANOVA, TMP increasing rate and operating cost regression models
were shown to be significant in all 1st order terms, 2nd order terms,
and interaction terms (p ¼ 0.05) in which each coefficient was also
significant (p < 0.05). Coefficient of determination (R2) of TMP
increasing rate and operating cost regression models were both
very high at 94.57% and 99.77%, respectively and the prediction of
response values deduced through regression models was expected
to show high accuracy. For TMP increasing rate, influence of 1st
order terms were larger than 2nd order terms and interaction
terms, and it was deducted that change of X2 among 1st order
terms showed most influence on the result values. In the case of
operating cost, influence of 1st order terms and 2nd order terms
were larger than interactions terms, and X1 and X21 had high in-
fluence on result values. As result of lack-of-fit test, p value of the
TMP increasing rate regression model was 0.634 and p value of the
operating cost regression model was 0.811. The null hypothesis
‘Occurred change is 0 because the regression model is not suitable’
was selected because both regression models were not significant
(p > 0.05). Thus, the influence of high-order terms, which were
Fig. 6. Fluorescence EEM of organic matter desorbed by (a) NaOCl, (b) NaOH - Organic
removed during the deduction of regression models, on response
matter desorption by NaOCl showed highest peaks at 360e400 nm/230e260 nm
(emission/excitation) and 430e470 nm/230e250 nm (emission/excitation). Organic
matter desorption by NaOH showed minor peak that was evenly distributed in the
whole domain of organic matter in addition to a main peak at 390e480 nm/
230e240 nm (emission/excitation). Red color is higher in concentration than green
color. (For interpretation of the references to colour in this figure legend, the reader is
referred to the web version of this article.)

operating cost and TMP increasing rate were selected as response

variables and optimization was performed to minimize the two
response variables. Optimized operating factors were chemical
interval, concentration, and duration to which these independent
variables were coded [
1, 1]. Ranges of coded operating variables
are shown in Table 2. Ranges of EFM operating conditions were set
with maximum values and minimum values recommended by the
vendor.
CCD was used to determine the regression models of the
response variables in which a total of 20 experiments were
designed. According to the order of designed tests, the plant was
operated to deduce actual data. Designed experiments and exper-
imental data from plant operation are shown in Table 3.
Multiple response surface design analysis was conducted based
on experimental data in which quadratic regression models on Fig. 7. FT-IR spectra of the organic matters desorbed by the NaOCl and NaOH. Both
chemicals display a clear stretch peak at wavelength of nearly 1650 cm
1, and a bend
operating cost (Eq. (6)) and TMP increasing rate (Eq. (7)) were
peak at a wavelength of 400e800 cm
1. An overtone/combination weak peak is
determined. observed at a wavelength of nearly 2000 cm
1.
1132 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134
Table 3
Ranges of operating conditions coded.
Independent variables Ranges of independent variables

1 0 1
Cleaning interval (X1) 1 3.5
Duration time (X2) 10 50
Chemical concentration.(X3) 100 300
values was minor, and the determined regression model was
considered valid. Also, as result of residual analysis, both regression
models statistically followed normal distribution and did not show
tendency because residuals were randomly distributed following
test order. A comparison between experimental data and data
predicted by the regression model, showed them to be almost
identical as shown in Fig. 8, in which RMSE showed very low values
of 0.67 and 0.425E-3. Therefore, the suitability of determined
regression models was considered as high and multiple response
surface optimization was conducted to deduce operating condi-
tions that minimize operating cost and TMP increasing rate.
Results of multiple response surface optimization are shown in
Fig. 9. Preference of operating cost and TMP increasing rate were
each 0.963 and 0.932, with an average of 0.948. Satisfactory results
were deduced as preference was close to 1. The optimal EFM
Fig. 8. Comparison between the experimental data and predicted data by the
regression model: (a) operating cost and (b) TMP increasing rate.
7
90
500
Fig. 9. Optimization results of the operating conditions.
Fig. 10. CO2 emission of the vender recommended and optimized conditions by the
LCA.
operating condition obtained was 6.3 d interval, 500 ppm con-
centration, and 76 min duration, in which the expected operating
cost was $0.121/m3 and the TMP increasing rate was 2.021% (see
Fig. 10).
3.4. Operating cost
The optimal operating conditions of EFM determined through
the newly proposed protocol are presented in Table 4.
The critical flux for irreversibility determined as the permeate
flux was 100 l m
2 h
1, which was higher than the vendor rec-
ommended permeate flux of 80 l m
2 h
1. The optimal chemical
reagent selected by examining the permeability restoration ratio
and irreversible foulant was NaOCl, the same as the vendor rec-
ommended chemical. The operating conditions of EFM determined
using RSM were 6.3 d interval, 500 ppm concentration, and 76 min
duration, which represented an increase of 4.3 d, 300 ppm, and
36 min, respectively, compared to the vendor recommended
conditions.
In order to investigate the cost reduction as a result of the
operating condition optimization, the pilot-scale plant was oper-
ated for 2 months (The data is not shown in this paper). The
operation determined that CIP interval was 47 d, an increase of 47%
compared to the vendor recommended interval of 33 d. In addition,
chemical cost, energy cost, and sludge disposal cost were calculated
and results are presented in Tables 5 and 6.
 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134 1133

Table 4 emission by chemical use, energy use, and sludge disposal was
Central Composite Design of operating conditions coded in operating cost and TMP 0.195 g CO2/m3, 112.241 g CO2/m3, and 0.314 g CO2/m3, respectively.
increasing.
It was calculated that energy use, i.e. CO2 emission by electricity use
Factors Operating cost ($/m3) TMP increasing (%) occupied over 99% of the total emission and that as a result of
Run X1 X2 X3 Predicted Experimental Predicted Experimental optimization, CO2 emission was reduced by about 26.5%, like in
operating cost. Based on this result, it is considered to be most
1 0 0 1 0.12446 0.12421 3.75279 2.45614
2 0 0 0 0.12392 0.12392 3.64434 3.50877 effective to develop a low energy operating system in water
3
1
1 1 0.13774 0.13745 6.43242 7.28070 treatment field, to reduce carbon dioxide.
4 1
1
1 0.12001 0.11959 11.55522 11.40351
5 0 0 0 0.12392 0.12392 3.64434 3.68421
6 0 0 0 0.12392 0.12392 3.64434 3.24561 4. Conclusions
7 1
1 1 0.12022 0.12007 10.12539 9.64912
8 0
1 0 0.12142 0.12256 7.40192 7.89474 This study investigated the operating cost and CO2 emission
9 0 1 0 0.12643 0.12528 1.57736 0.96491
reduced by optimizing the operating conditions for chemical
10
1 0 0 0.14153 0.14152 2.13876 1.31579
11 0 0 0 0.12392 0.12392 3.64434 4.64912 cleaning used to improve the membrane filtration process. A new
12 1 0 0 0.12050 0.12051 5.52472 6.22807 protocol that can be easily used in the field was proposed. Opti-
13 0 0 0 0.12392 0.12392 3.64434 3.59649 mization of operating conditions for EFM was tested using a pres-
14 0 0
1 0.12340 0.12364 5.84051 7.01754
surized UF membrane facility currently in operation. In addition, a
15 0 0 0 0.12392 0.12392 3.64434 3.42105
16 1 1 1 0.12115 0.12143 2.32715 3.07018
pilot plant was operated under the optimized operating conditions
17
1 1 1 0.14711 0.14753 0.25698 0.43860 identified to compare costs of operation, energy, chemicals, and
18
1
1
1 0.13612 0.13585 6.85347 6.14035 sludge disposal.
19 1 1
1 0.12065 0.12094 6.08154 5.26316 A flux-stepping test was performed with a modified flux-step
20
1 1
1 0.14520 0.14536 3.00259 3.50877
method to determine the permeate flux. Ftot and Rrev rapidly
increased from 100 l m
2 h
1, while Firr and Rirrev rapidly increased
from 120 l m
2 h
1. Based on the analysis, the critical flux for
Chemical cost was reduced by 37.5% from $0.0030/m3 to irreversibility was selected as 100 l m
2 h
1, and the existing
$0.0019/m3. Cost was reduced despite an increase in the chemical vendor recommended flux of 80 l m
2 h
1 was determined as the
concentration used by 2.5 times, due to prolongation of the interval threshold flux.
by over three times. Energy cost was reduced by 22.5% from The permeability recovery rate and irreversible foulant of
$0.1479/m3 to $0.1142/m3. The effect of operating time saved by chemicals were examined to select an appropriate chemical for the
increasing the permeate flux is larger than the cost incurred by the cleaning. It was found that major irreversible foulants were organic
use of a permeate pump. Sludge disposal cost was reduced by 75% as the permeability recovery rate of NaOH and NaOCl was higher,
from $0.0105/m3 to $0.0026/m3. As a result, the total operating cost while that of citric acid was low. The examination of the irreversible
was $0.1187/m3, which is 26.5% lesser compared to the operating foulant through FEEM and FTIR also confirmed that major foulants
cost under a vendor recommended setup, and similar to the were the organic materials like humic acid that have aromatic and
amount predicted by the regression model. This study found that alkene functional groups. Thus, NaOCl, which is specialized in
the effect of operating cost savings achieved through optimization removing organic materials such as humic acid was selected as the
of operating condition for chemical cleaning was excellent. In appropriate chemical.
addition, the effect of saving initial investment costs, such as the The operating conditions of EFM including chemical interval,
decrease of modules due to membrane life and an increase in the duration and concentration, were optimized through RSM. Re-
filtration flux from optimization, were not included. If these factors sponses were the operating cost and TMP increasing ratio, and
are additionally considered, the operating cost savings would be regression models for the responses were developed. The regres-
much higher. sion models were fit based on validity tests including t-test,
When the membrane filtration process was operated in the ANOVA, and lack-of-fit test. The result of multiple response surface
vender recommended condition, CO2 emission by chemical use, optimization showed that the operating cost and the TMP
energy use, and sludge disposal was 0.311 g CO2/m3, 145.439 g CO2/ increasing rate were minimized at an interval of 6.3 d, concentra-
m3, and 1.245 g CO2/m3, respectively and when the membrane tion of 500 ppm, and duration of 76 min. In this setting, the ex-
filtration process was operated in the optimized condition, CO2 pected operating cost was $0.121/m3, and the TMP increasing rate

Table 5
Comparison of operating factors between vendor recommended conditions and optimized condition.

Type Operating conditions

Permeate flux (l m
2 h
1) Chemical reagent Interval (day) Concentration (ppm) Duration (min)

Vendor recommended conditions 80 NaOCl 2 200 40

Optimized conditions 100 NaOCl 6.3 500 76

Table 6
Comparison of unit cost ($/m3) between the vender recommended and optimized conditions.

Operating cost ($/m3)

Chemicala Energyb Sludge disposalc Total

Vender recommended conditions 0.0030 0.1479 0.0105 0.1615

Optimized conditions 0.0019 0.1142 0.0026 0.1187
Saving rate (%) 37.5 22.8 75.0 26.5
1134 S.S. Yoo et al. / Journal of Environmental Management 206 (2018) 1126e1134
was 2.021%.
A pilot-plant was operated for a long-term under the optimal
operating conditions, and operating cost and CO2 emission were
calculated. The calculated operating cost and CO2 emission were
$0.1187/m3 and 112.75 g CO2/m3, a reduction of approximately
26.5% compared to the operating cost and CO2 emission under the
vendor recommended conditions. Thus, the effect of operating
cost and CO2 emission reduction from optimization of chemical
cleaning was excellent. In addition, the calculation of operating
cost in this study did not include the effect of saving initial in-
vestment costs, such as the decrease in the number of modules
and reduction in installation area, due to the change in the cycle of
membrane replacement and the increase of the permeate flux
from the change in the operating conditions. Thus, the operating
cost reduction with the optimization of chemical cleaning was
actually much higher. This effect will be reflected in a planned
future study.
Funding
This research did not receive any specific grant from funding
agencies in the public, commercial, or not-for-profit sectors.
Conflict of interest
We wish to confirm that there are no known conflicts of interest
associated with this publication and there has been no significant
financial support for this work that could have influenced its
outcome.
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