DES-12620; No of Pages 9

Desalination xxx (2015) xxxxxx

Contents lists available at ScienceDirect

Desalination
journal homepage: www.elsevier.com/locate/desal

Organic fouling and reverse solute selectivity in forward osmosis: Role of working
temperature and inorganic draw solutions
Jiyong Heo a, Kyoung Hoon Chu b, Namguk Her a, Jongkwon Im b,c, Yong-Gyun Park d, Jaeweon Cho e,
Sarper Sarp f, Am Jang g, Min Jang h, Yeomin Yoon b,
a

Department of Civil and Environmental Engineering, Korea Army Academy at Young-Cheon, 135-1 Changhari, Kokyungmeon, Young-cheon, Gyeongbuk 770-849, South Korea
Department of Civil and Environmental Engineering, University of South Carolina, Columbia, SC 29208, USA
National Institute of Environmental Research, Environmental Research Complex, 42 Hwangyeong-ro, Seo-Gu, Incheon 404-170, South Korea
d
Environmental Process Design Team, GS E&C, 33 Jongro, Jongro-gu, Seoul 110-702, South Korea
e
School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST),UNIST-gil 50, Ulju-gun, Ulsan 689-798, South Korea
f
Qatar Environment and Energy Research Institute, Qatar Foundation, Education City, CP4, PO Box: 5825, Doha, Qatar
g
School of Civil and Architecture Engineering, Sungkyunkwan University, 2066 Seobu-ro, Jangan-16 Gu, Suwon, Gyeonggi-do 440-746, South Korea
h
Department of Civil Engineering, Faculty of Engineering, University of Malaya, Kuala Lumpur 50603, Malaysia
b
c

H I G H L I G H T S
We examined the inuence of high levels of organic foulants on FO membrane performance.
We evaluated the inuence of temperature on the forward water and reverse salt ux behavior.
Lower water viscosities played a dominant role in enabling concentrative internal concentration polarization.

a r t i c l e

i n f o

Article history:
Received 31 March 2015
Received in revised form 16 June 2015
Accepted 16 June 2015
Available online xxxx
Keywords:
Forward osmosis
Unpressurized pressure-retarded osmosis
Fouling
Temperature
Inorganic draw solutions
Reverse solute ux selectivity

a b s t r a c t
The water ux of several draw solutions (DSs, solutes: KCl, NaCl, CaCl2, Na2SO4) and fouling propensity of two
different organic foulants (humic acid and alginate) were systematically investigated using forward osmosis (FO)
and unpressurized pressure-retarded osmosis. In addition, reverse solute selectivity was evaluated to characterize
the water and salt transport mechanisms at different temperatures and in the presence of four different inorganic
DS compounds. The inuence of solution viscosity has signicant implications in FO applications, because the water
molecules easily penetrated and diffused throughout the FO membrane active layer (AL) and supporting layer (SL)
with increasing temperatures, which is mainly correlated with the lower water viscosities with increasing temperatures. The results indicated that the water ux on average signicantly increased from 9.5 to 13.7 and 24.9 LMH
when the operating temperature was increased from 5 to 20 and 45 C, which corresponded to a 44 and 262% increase in the water ux, compared to the FO mode at 5 C. However, the water ux and viscosity exhibited generally
constant trends with respect to the elevating temperature. In addition, elevating temperature increased the reverse
solute ux selectivity (RSFS), not only by decreasing the internal concentration polarization (the AL and SL) and the
wettability within the effective porosity of the SL, but also via the improvement of water molecule diffusion kinetics
rather than solute diffusion. In addition, the RSFS was inversely related to the solute permeability of the different
DSs and followed the order Na2SO4 N CaCl2 N NaCl N KCl. These results have signicant implications for the prediction of water ux behavior and the selection of DSs at different temperatures in osmotically driven FO processes.
2015 Elsevier B.V. All rights reserved.

1. Introduction
Osmotically driven membrane processes (ODMPs) involve spontaneous water movement by means of a natural chemical gradient in which a
solution tends to move from a state of lower osmotic pressure to one
higher osmotic pressure through a semi-permeable membrane. ODMPs
Corresponding author.
E-mail address: yoony@cec.sc.edu (Y. Yoon).

have great potential in sustainable water purication, since they reduce

the energy required for seawater desalination and typically exhibit low
propensities for membrane fouling [13]. A number of ODMPs, including
forward osmosis (FO) and pressure-retarded osmosis (PRO), have been
studied [1,416]. Prior studies have focused on (i) understanding internal
and external concentration polarization (ICP and ECP, respectively),
which reduce the deleterious effects of the water ux [4,7]; (ii) membrane fabrication techniques for higher water ux environments [11,17,
18]; (iii) module development with feed solutions (FSs) containing

http://dx.doi.org/10.1016/j.desal.2015.06.012
0011-9164/ 2015 Elsevier B.V. All rights reserved.

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

various foulants and scalants [6,9,10,1416,19]; and (iv) development of

possible organic and inorganic draw solutions (DSs) based on reverse salt
diffusion [8,12,13]. In these studies, the performance of ODMPs was inuenced by the following temperature-dependent factors [13,2023]:
membrane properties, solution properties, module conguration,
and operating conditions. Particularly, the temperature directly
inuenced the thermodynamic characteristics of the FSs and membrane properties [2426], which, in turn, directly inuenced the
water permeability, salt permeability, and reverse solute ux selectivity
(RSFS) [13,21].
Signicant temperature variations have been observed in several
practical membrane separation applications, including municipal and
industrial feed water purication [20,22,25,26]. These temperature
variations inuence the key characteristics of membrane separation
processes, such as solute mass transfer, water movement, concentration
polarization (CP), and membrane fouling, which are strongly inuenced
by changes in solution viscosity, foulant characteristics, water diffusivity, and osmotic pressure. For example, the viscosity of water and solute
rejection decrease with increasing feed water temperature; in contrast,
solute diffusivity and solution osmotic pressure increase with increasing
feed water temperature, thereby leading to a greater water ux at higher
temperatures [22]. Thus, CP can be reduced at higher feed water temperatures by enhancing salt transport in the membrane support layer (SL),
which, in turn, affects the solute passage and osmotic pressure during
the membrane separation process. With respect to membrane fouling, increasing the temperature typically leads to a decrease in humic acid (HA)
colloids, which decrease specic cake resistance and result in more
porous deposits on the membrane surface [26]. In addition, biolm formation is enhanced at higher temperatures, particularly when wastewater is used as the FS.
The inuence of temperature on FO membrane processes has also
been studied by evaluating reverse solute diffusion as a function of
water permeation. For example, Phillip et al. [13] demonstrated that the
reverse ux selectivity was not dependent on the membrane structural
characteristics or the bulk DS concentrations for organic and inorganic
solutions. However, the reverse ux selectivity was dependent on the selectivity of the active layer (AL) and the osmotic pressure, both of which
varied with temperature [8,13]. The inuence of working temperature on
FO separation performance was studied by Zhao et al. [20], who demonstrated that higher temperatures favor higher initial uxes, water recoveries, and concentration factors; however, greater membrane scaling was
observed when the FS was introduced at temperatures of 25, 35, and
45 C. You et al. [23] reported that the mass diffusion kinetics, such as
the water trans-membrane ux in the FO process, could be improved
signicantly by increasing the temperature. In the temperature range of
20 to 45 C, the FO ux positively correlated with the water ux and
bulk solution temperature. Xie [21] recently reported the inuence of
temperatures between 20 and 40 C on NaCl RSFS. In practical terms, increasing the temperature contributed to an increase in pure water and
NaCl permeability coefcients, thereby suggesting that higher temperatures signicantly increased solute diffusivity and decreased water
viscosity. Moreover, in the Xie's study, the RSFS did not change with
increasing temperature, which suggested no change in membrane
properties.
Relatively little is still known about the inuence of increasing
temperature on the correlation of water ux and solution viscosity,
RSFS, and FO membrane fouling propensity in the presence of different
inorganic DSs in FO- and PRO-mode operations. Therefore, in the study
reported herein, the specic objectives of the research included the
following: (i) examination of the inuence of high levels of organic
foulants (i.e., 60 mg L1 of HA and alginate) and secondary efuents
on the fouling characteristics of FO membranes at various temperatures
(5, 20, and 45 C) in both FO and unpressurized PRO (uPRO) modes; (ii)
evaluation of the inuence of increasing temperature (5 up to 45 C) on
the forward water ux and reverse salt ux behavior (i.e., the solution
viscosity and solute selectivity coefcients); and (iii) determination of

the inuence of temperature on the RSFS and FO membrane properties,

which was evaluated using previously studied reverse draw solute permeation modeling. This systematic assessment of temperature inuence will improve the understanding of fouling propensity, forward
water, and reverse solute ux behavior and enable better selection of
DSs for osmotically driven FO processes.
2. Materials and methods
2.1. FO membranes and characterization
Commercially available at-sheet cellulose triacetate (CTA) FO
membranes were obtained from Hydration Technologies, Inc. (Albany,
OR, USA). These FO membranes were developed specically to exhibit
unique characteristics (e.g., greater hydrophilicity and less ICP) compared
with other semi-permeable membranes. The ICP was reduced through
the use of a thin, synthetic, asymmetric CTA AL; embedded ultrathin polyester woven mesh SLs were incorporated for mechanical strength [27].
CTA content in the membrane was conrmed by Fourier-transform infrared (FTIR) spectroscopy (Fig. S1); the higher frequency peak at
1737 cm1 associated with acetyl functional groups of CTA was detected
on the membrane surface. After it was cut to the desired size, the FO
membrane was preserved by soaking in deionized (DI) water and stored
away from direct sunlight in a refrigerator at 4 C. According to the supplier, the membrane exhibited 99.4% salt rejection and an overall tap
water ux of 7.7 and 12.0 L m2 h1 (LMH) in the FO and uPRO
modes, respectively. The electrophoretic mobility of an FO membrane
was less negative than the surface potential; the zeta potential (ZP)
ranged from 4 to 8 mV. The water contact angles of the FO membrane selective layer (or AL) and the back layer (or SL) were 61.3
0.8 and 66.4 1.3, respectively. More details with respect to membrane
properties are provided separately [28].
2.2. Feed and draw solutions
Sodium alginate (SA, SigmaAldrich, St. Louis, MO, USA) and HA
(SigmaAldrich, St. Louis, MO, USA) were used as model organic
foulants for polysaccharides and natural organic matter (NOM), respectively. These organic macromolecules are the major cause of organic
fouling during membrane ltration of surface water, seawater, and
wastewater efuent. To ensure the consistency of the organic composition in the FS, stock solution was prepared by concentrating SA and HA.
SA has been widely used in membrane fouling studies to simulate
wastewater efuent organic matter containing high levels of soluble
microbial products. SA was received from the manufacturer in powder
form with a 1280 kDa molecular weight; a 2 g L1 stock solution of
SA in DI water was prepared. HA, which is a mixture of complex polyelectrolytes with carboxylic and hydroxyl functional groups, has
been used extensively as a model organic foulant for high molar mass
NOM, and its characteristics can be found elsewhere [29]. HA stock
solution was prepared by dissolving in DI water and then sequentially
ltering through GF/F (0.7-m) glass microber lters (Whatman Inc.,
Piscataway, NJ, USA) and Durapore (0.45 m) membrane lters
(Millipore Inc., Billerica, MA, USA) to remove any impurities and particulate matter. Stock solutions were stored in sterilized glass bottles at
4 C and used in subsequent experiments. The molecular weights of
the HA were about 15 kDa, as outlined in our previous study [30]. A
total organic carbon (TOC) analyzer (Shimadzu, Corp., Kyoto, Japan)
was used to measure the organic carbon contents of the stock solutions
and FSs.
The FS for the FO experiments was prepared by further dilution of SA
and HA stock solution with DI water to obtain a desired concentration of
60 mg L1 dissolved organic carbon (DOC). The ionic strength of the FS
was adjusted by adding NaCl to maintain a nal background ionic
strength of 1 mM. The pH was adjusted to 6.5 by addition of 0.1 M
NaOH and 0.1 M HCl, as needed. DS was prepared by dissolving different

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

concentrations of various inorganic compounds (NaCl, Na2SO4, CaCl2, or

KCl) (SigmaAldrich, St. Louis, MO, USA) in DI water. These four inorganic
compounds were chosen as DS solutes, since their thermodynamic properties are well established.

2.3. Bench-scale FO set up

The FO experiments were conducted with an in-house, bench-scale
stainless-steel plate and frame as an FO cell coupled with an FS and a DS
tank. The setup was built with symmetric, rectangular double-channels
on both sides of the membrane to enable simultaneous owing of the FS
and DS; the channel dimensions were 76 mm 27 mm (length
width), providing an effective membrane coupon area of 41.04 cm2.
Fig. S2 shows the schematic diagram of the bench-scale FO system
used in these experiments. The design and operating details for the FO
system have been recently reported elsewhere [28]. Each set of each
experiment were carried out for more than 12 h: FO-mode runs
were initiated with DI water as FS to the membrane active layer
and a 1 M NaCl DS; uPRO-mode runs were initiated with DI water
as FS to the membrane support layer and a 1 M NaCl DS. The ionic
strength of the FS was maintained at a NaCl concentration of 1 mM.
The solution temperature was varied from 5 to 45 C, and was controlled to within 1.5 C using a water heater/chiller (Fisher Scientic
Isotemp Chillers, Pittsburgh, PA, USA) throughout the baseline and
fouling tests. Mesh spacers were employed to support the FO membrane at a constant ow rate of 0.19 L min 1 (corresponding to a
cross ow velocity of 9.8 cm s1) for the FS and DS. Flow rates were
monitored using ow meters (Dwyer, Michigan City, IN, USA) during
all experiments.

2.4. FO membrane fouling experiments and reverse salt selectivity

The FO fouling experimental protocol included the following steps.
First, a new membrane coupon was placed where the CTA membrane
was sandwiched in the unit cell, as described previously. Next, the system was thoroughly rinsed with DI water, and concurrent cross-ows of
DI water solutions were maintained for more than 1 h to stabilize the
system. At this stage, the FS with 60 mg L1 DOC (foulant) was introduced via the feed reservoir described above. To achieve a water ux,
1 L of a 2 M NaCl stock solution was added to the DS tank. Both the DS
and FS were continuously mixed using a magnetic stirrer. The DS reservoir was placed on a digital balance (AV8101, Ohaus, NJ, USA), and the
water ux in the DS was recorded by monitoring the weight change of
the DS; the weight data were automatically logged into a computer
every 10 min. Prior to each main experiment, baseline experiments
were conducted to quantify the ux decline associated with declining
osmotic driving as the DS was gradually diluted by the permeate
water. Baseline experiments also enabled correction of the ux
curves obtained during fouling runs, and they enabled direct comparison of the fouling and temperature effects and quantication of
NaCl reverse diffusion from DS to FS, even when no foulant was added
to the FS.
To quantify the reverse solute ux during the FO experiments, the
solute concentration in the FS was monitored at 3-min intervals using
a calibrated conductivity meter with a cell constant of 1 cm1 (Thermo
Scientic, Vernon Hills, IL, USA). These measurements enabled the
determination of the pure water permeability of the membrane AL, A,
the solute permeability of the membrane AL, B, and the structural
parameter of the membrane SL, S, by treating A, B, and S as adjustable
parameters to enable simultaneous tting of experimental water and
reverse salt ux data to corresponding governing equations, as described in our recent publication [28]. Some runs were duplicated to
conrm the reproducibility of the FO fouling and temperature effect
experiments.

3. Results and discussion

3.1. FO membrane characterization
The intrinsic properties of FO membranes were investigated by
calculating the selectivity of the dilutive ICP of the AL of FO membranes
based on the solution-diffusion (SD) model approach. The membrane
selectivity is related to the ratio of A to B, where A is the intrinsic pure
water permeability coefcient and B is the intrinsic salt permeability
coefcient of the FO membrane AL. The parameters for determining
the selectivity coefcient are similar to those presented in a previous
study based on the reverse osmosis (RO) mode [7,31]. Although accurate prediction of the characteristic transport parameters of hydrophilic
FO membranes is difcult using the SD model, the inherent discrimination of RO- and FO-mode parameters enabled determination of the FO
membrane characteristics with different DS solutes. The selectivity
values were calibrated using the data determined experimentally from
RO-mode and previously described methods [28]. Briey, the selectivity
values (A/B) were determined using a pressurized, dead-end conguration mode with a stirring speed of 300 rpm. To determine A and B, the rejection of inorganic salts and the pure water ux in the RO mode were
plotted vs. applied pressure based on the SD model approach.
The FO membrane water permeability coefcient (A) was
0.517 L m2 h1 bar1, which is slightly higher than that reported in
our previous research. The difference was attributed to the variation
between experimental protocols and membrane coupons. Fig. S3
shows the membrane selectivity (A/B) for the four types of draw solutes
investigated in this study. The A/B values followed the order
Na2SO4 N CaCl2 N NaCl N KCl. The determination of A and B for the FO
membrane coupon and the four types of draw solutes (i.e., the solute
mass transfer properties of the FO membrane and the DS solute ions)
elucidated the trends in solute permeation through the FO membrane
[32]. KCl exhibited the highest membrane selectivity, despite the smaller
size of the cation Na+ compared with the cation K+. However, K+ cations are less hydrated than Na+ cations, leading to greater permeability
of K+ through the FO membrane compared with Na+. This result conrms the higher solute transfer of KCl than that of NaCl based on solution
electro-neutrality. In addition, the membrane selectivity was greater in
divalent salts than in monovalent salts. The A/B values of divalent salts
(7.93 0.13 and 9.24 0.57 bar1 for CaCl2 and Na2SO4, respectively)
were approximately 3.54.0 times higher than the membrane selectivity
of the monovalent salts (A/B values of 2.65 0.28 and 2.27 0.13 bar1
for NaCl and KCl, respectively). The higher solute permeability of NaCl
and KCl was attributed to the smaller hydration radii of Na+
(0.358 nm), K+ (0.331 nm), and Cl (0.332 nm) compared to those of
Ca2+ (0.421 nm) and SO24 (0.379 nm), indicating that the divalent
salts have better separation properties than the monovalent salts in the
FO membrane.

3.2. Effects of solution temperature and FO membrane orientation on water

ux and organic fouling
As indicated by the Van't Hoff equation, temperature directly inuences the osmotic pressure of the solution and other thermodynamic
properties, such as diffusion coefcient, viscosity, etc [13,20,22]. Since
the FO process involves two independent streams between feed and
draw solutions on each side of the membrane, the inuence of temperature on each solution may be inuenced by the FO membrane orientation (FO vs. uPRO). The inuence of temperature and membrane
orientation on the organic fouling and water ux were evaluated in
the FO experiments using isothermal FS and DS temperature stages
and solution temperatures of 5, 20, and 45 C. Fig. 1 shows the inuence
of temperature on the pure water ux (baseline, using DI water as feed)
and water ux (using 60 mg L1 HA or SA as foulants) in the FO process
at different membrane orientations (FO and uPRO modes).

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

d
18

10

15

Water flux (L m h )

12

-1

-2

-2

-1

Water flux (L m h )

6
4
Baseline - DI
-1
Feed - HA (C 0 = 60 mg L as DOC)

12
9
6
Baseline - DI
-1
Feed - HA (C 0 = 60 mg L as DOC)

-1

-1

Feed - SA (C 0 = 60 mg L as DOC)

Feed - SA (C 0 = 60 mg L as DOC)

0
0

10

12

14

15

25

Water flux (L m h )

30

12

14

-1
-2

-2

12
9
6
Baseline - DI
Feed - HA (C 0 = 60 mg L -1 as DOC)

20
15
10
Baseline - DI
Feed - HA (C 0 = 60 mg L -1 as DOC)

-1

Feed - SA (C 0 = 60 mg L -1 as DOC)

Feed - SA (C 0 = 60 mg L as DOC)

0
0

10

12

Time (hr)

10

12

Time (hr)

f
50

25

40

-1

Water flux (L m h )

30

-2

-1
-2

10

e
18

-1

Water flux (L m h )

Water flux (L m h )

Time (hr)

Time (hr)

20
15
10
Baseline - DI
Feed - HA (C 0 = 60 mg L -1 as DOC)

30
20
Baseline - DI
Feed - HA (C 0 = 60 mg L -1 as DOC)

10

Feed - SA (C 0 = 60 mg L -1 as DOC)

Feed - SA (C 0 = 60 mg L -1 as DOC)

0
0

10

12

Time (hr)

10

Time (hr)

Fig. 1. Pure water ux (baseline, using DI water as feed) and water ux (using 60 mg L1 HA or SA as foulant) with various temperatures at different membrane orientations: (a) 5 C,
(b) 20 C and (c) 45 C in the FO mode and (d) 5 C, (e) 20 C and (f) 45 C in the uPRO mode. Operating conditions: pH = 6.5; ionic strength = 1 mM; and NaCl = 2 M.

As shown in Fig. 1, the water ux improved signicantly when the

temperature of both of the solutions was increased from 5 to 45 C.
When the operating temperature of both of the solutions was increased
from 5 to 20 and 45 C, the water ux (baseline) increased from 9.5 to
13.7 and 24.9 LMH, respectively. These increases corresponded to a 44
and 262% increase in the water ux, respectively. The temperature
signicantly inuenced the magnitude of the water ux in the FO
mode, since it greatly reduced the ICP across the membrane. The increase in the water ux at higher temperatures was attributed to changes in thermodynamic properties, such as the osmotic pressure, diffusion
coefcient, and/or the viscosity of the FS and DS. As the temperature
was increased from 5 to 20 and 45 C, the osmotic pressure increased
(data not shown: however, the data is available on request), which
was expected to increase the net driving force and, hence, enhance
the water ux during the FO process. In addition, the water viscosity
decreased, thereby resulting in an increase in the water self-diffusivity
at higher temperatures, which, in turn, resulted in an increase in the
mass transfer via reducing the inuence of ICP.

Similar increasing trends in the water ux were observed in the

uPRO mode. With an increase in temperature from 5 to 20 and 45 C,
the pure water ux (baseline) increased from 15.1 to 25.9 and 41.4
LMH, respectively. The increase in the water ux in the uPRO mode
was related to both thermodynamic properties and the ICP phenomenon in the membrane support layer. The temperature variation inuenced the water ux, which inuenced the thermodynamic properties
(i.e., the water viscosity and diffusivity). A lower driving potential
(membrane ux) was observed with increasing DS concentration as a
necessary consequence of dilutive ICP in the membrane SL in the FO
mode [27,33], which was also inuenced by the temperature variations.
As shown in Fig. 2, water molecules easily passed and diffused through
the AL and SL of the FO membrane upon increasing the temperature in
the uPRO mode. As a result, increasing the temperature from 5 to 20
and 45 C generated an increase in the water ux of 72 and 274%, respectively, in the uPRO mode.
Organic fouling in the FO and uPRO modes was evaluated using single
foulants (60 mg L1 of HA and SA). According to the literature, a

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

Normalized flux Jw/Jw,0 (%)

a
FO mode
uPRO mode

Humic acid
100
90
80
70
60

20

45

Normalized flux Jw/Jw,0 (%)

b
FO mode
uPRO mode

Sodium alginate
100
90
80
70
60

20

45

Fig. 2. Comparison of normalized water ux for (a) humic acid and (b) sodium alginate in
the FO and uPRO modes with respect to the temperature. Operating conditions: pH = 6.5;
ionic strength = 1 mM; and NaCl = 2 M.

maximum foulant concentration of 60 mg L1 simulates the efuent

organic matter of wastewater [15,34,35]. The two different foulants
were used to investigate two different characteristics of fouling; HA is
more hydrophobic than SA. Experiments were carried out over more
than 12 h to thoroughly evaluate the foulant effects. The inuence of temperature variation on organic fouling was also investigated; hydrodynamic shear was enhanced by decreasing viscosity with respect to
increasing temperature. The results of fouling runs in the FO and uPRO
modes, with temperature variations from 5 to 45 C, are shown in
Fig. 2; decreases in the ux percentage after fouling are presented as

normalized uxes in this gure. In the normalized ux decline (comparing between foulant and temperature effects), SA fouling at lower
temperature conditions was the most pronounced, followed by middle
and higher temperature conditions.
In the uPRO mode, low temperatures caused more severe fouling,
based on the observed changes in the solution characteristics (water
viscosity) and fouling patterns. The fouling propensity was more severe
at low temperature because the viscosity of an alginate solution was
variable with temperature (decreasing temperature resulting in increasing viscosity), and also the longer chins can be formed at higher
viscosities even similar concentrations of alginate solution. In addition,
the more severe SA fouling and ux decline with decreasing temperature was also attributed to cake layer formation [10,15], which is the
formation of a cake-enhanced, cross-linked, thick gel layer on the membrane surface. A schematic description of this change for the temperature is depicted in Fig. 3. The fouling rate increased with the volume
concentration factor (VCF), as shown in Fig. S4. The VCF provides a
more reasonable comparison of the organic fouling and ux decline
than the permeate volume or time, since the concentration of retained
organic foulants on the membrane surface in the FS was highly variable
with respect to the condensing volume. This variability signicantly inuenced the physical and chemical properties of the membrane and solute at the interface of the membrane. Expressed as VCF (VCF = 1.03.0,
corresponding to a recovery of 058.7%), the fouling resistance was signicant with respect to SA at low temperatures, with water ux losses
of about 30.2% compared with the baseline experiments.
Fouling experiments at different temperatures were also conducted to
evaluate the inuence of membrane orientations, namely, the AL facing
the FS in the FO mode and the SL facing the FS in the uPRO mode.
Fig. S5 compares the average water ux proles in the FO and uPRO
modes for the HA and SA organic foulants (at a loading of 60 mg L1).
Generally, greater ux reduction was observed with SA. In the FO mode,
the water uxes at the end of 20 h test runs in the absence of SA at different temperatures (5, 20, and 45 C) were 9.5, 13.7, and 24.9 LMH, respectively, while those in the presence of SA exhibited lower water ux values
of 8.6, 12.7, and 21.9 LMH, respectively. In the uPRO mode, the ux reduction was 24% greater, with a water ux of 25.9 and 19.8 LMH at 20 C in
the absence and presence of 60 mg L1 of SA, respectively. In general,
the water ux dropped by more than 14.9 and 30.2% compared with
baseline tests based on temperature variations in the uPRO mode. In
uPRO mode, more severe HA fouling were observed since the porous SL
is exposed to the foulant containing feed solutions, as shown in Fig. S6.
Thus, minimal ux decline was observed in experimental runs of more
than 12 h in the FO mode in the presence of both types of organic foulant

High Temperature

Low Temperature

Feed

Feed
m

eff

Draw

Active layer

Support layer

eff

Draw

Active layer
Support layer

Fig. 3. A conceptual illustration for the inuence of temperature on the uPRO membrane fouling and concentration polarization prole (m: osmotic pressure difference across the membrane,
eff: effective osmotic pressure).

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

divalent (CaCl2, Na2SO4) inorganic DS compounds in a simple matrix

with an AL-facing FS conguration for the optimal operating parameters
in FO desalination applications at different temperatures. In this conguration, the permeate water ux behavior with NaCl, KCl, and CaCl2 in
the FO membrane (average ux values of 8.43, 9.10, and 9.89 LMH,
respectively, at 20 C) was greater than that observed for Na2SO4 DS
(average ux of 7.11 LMH at 20 C), as shown in Fig. 4. In the FO mode,
the osmotic driving force resulting from the concentration difference
across the membrane and the osmotic pressure (based on theoretical
calculations) can be extremely high when using divalent inorganic compounds in the DS instead of monovalent inorganic compounds; the
osmotic pressures of 1 M NaCl, KCl, CaCl2, and Na2SO4 were 45.3, 44.8,
62.9, and 54.1 bar, respectively. Theoretically, divalent inorganic compounds have great potential for providing high water recovery and
water ux. However, the water ux was signicantly reduced. In this
study, all of the DS solutes studied exhibited a similar inuence on the
water ux behavior based on their respective osmotic pressure differences; however, the DS containing Na2SO4 exhibited the lowest water
ux behavior, even though this solute has the highest net bulk osmotic
pressure based on osmotic pressure calculations. This apparent discrepancy between observed and expected behavior was attributed to the different diffusivities of the divalent DSs, which were inversely proportional to
their osmotic pressures. Low water ux was thus observed, since the ICP
effect is inversely proportional to the solute diffusivity, which was greater
in the presence of larger divalent ions. The mass transfer of these DSs in
FO membrane follows an inverse order of the membrane selectivity
(A/B) except for CaCl2 because the ICP inuence is inversely proportional to the solute mass transfer. Thus, greater dilutive ICP in the SL induced
a loss of osmotic pressure in DSs with CaCl2 and Na2SO4 throughout the
entire ltration process. The ICP increase observed in the presence of divalent DSs resulted in a net osmotic pressure decrease in the osmotically driven FO process. However, the absolute viscosity of both FS and DS
decreased with increasing temperature, which enhanced the diffusivity
of the water ux through the membrane AL and porous layer, thereby

(HA and SA). The FO mode exhibited less fouling propensity to both
organic foulants than the uPRO mode. However, greater ux decline
was observed in the PRO mode in the presence of SA in the FS. The concentrative ICP (in the uPRO mode) exhibited higher ux and greater
ux decline in the porous membrane than the dilutive ICP (in the FO
mode), while the uPRO mode was not resistant to fouling on the membrane surface. This behavior was attributed to two processes: (i) The ICP
inuence (SA fouling can lead to the enhanced ICP) [10] and (ii) the
foulant layer roughness induced by the membrane orientations (uPRO
orientation was more prone to fouling). In the uPRO mode, the ICP was
less severe, but other factors, including greater membrane surface
porosity and rougher structure, resulted in rapid fouling and, consequently, greater ux decline. For example, more porous and rougher
membranes enabled greater pore blocking by foulants in the FS, leading
to foulantfoulant interactions and the initiation of cake layer formation
on the SL. These processes then promoted enhanced ICP and a reduction
in the differential osmotic pressure across the membrane, thereby leading
to a ux decline in the uPRO mode. As shown in Fig. 2b, SA did not cause
an obvious water ux loss in the FO mode throughout the ltration process. In contrast, greater ux reduction was observed after SA was introduced during the uPRO mode at low temperatures. This behavior was
attributed that the kinetics of SA sol/gelling process was favored in the
uPRO mode at low temperatures (i.e., the SA gels set more with low temperature) and the synergistic interactions between the higher solution
viscosity and denser cake layer formation (uPRO orientation was more
prone to SA fouling compared to the FO orientation) on the membrane
surface.
3.3. Effects of solution temperature on water ux behavior during the FO
process: The role of different types of draw solution
The FO water ux behavior in the presence of different DSs was systematically studied at different solution temperatures. FO-mode tests
were performed to evaluate the inuence of mono- (NaCl, KCl) and

b
1M KCl DS, 5 oC
1M KCl DS, 20 oC
1M KCl DS, 45 oC

20

-2

-1

20

Water flux (L m h )

25
1M NaCl DS, 5 oC
1M NaCl DS, 20 oC
1M NaCl DS, 45 oC

-2

-1

Water flux (L m h )

25

15
10
5
0

15
10
5
0

100

200

300

400

500

Permeate volume (mL)

c 25

100

200

300

400

500

Permeate volume (mL)

d 25
-1

Water flux (L m h )

20
15

1M Na2SO4 DS, 30 oC

20

1M Na2SO4 DS, 45 oC

-2

1M CaCl2 DS, 5 oC
1M CaCl2 DS, 20 oC
1M CaCl2 DS, 45 oC

-2

-1

Water flux (L m h )

1M Na2SO4 DS, 20 oC

10
5

15
10
5
0

0
0

100

200

300

Permeate volume (mL)

400

500

100

200

300

400

500

Permeate volume (mL)

Fig. 4. Permeate water ux behavior with various DSs of (a) NaCl, (b) KCl, (c) CaCl2, and (d) Na2SO4 at different temperatures in the FO membrane. Operating conditions: pH = 6.5 and
ionic strength = 1 mM; and NaCl = 2 M.

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

inducing a positive inuence on the water ux, as shown in Fig. 4. (All DSs
exhibited increased water ux with increasing FS and DS temperatures.)
3.4. Relating water viscosity to FO membrane water ux
The water ux is an important factor in FO membrane desalination
applications. The average water ux and multiple water viscosity data
were compared. The permeate ux is principally dominated by temperature; in this study, the experimental water uxes were signicantly increased by increasing the solution temperature, as shown in Fig. S7. This
result was attributed to several factors: uid viscosity, concentration
polarization, water self-diffusivity, and the mass transfer coefcient. In
this study, we isolated the inuence of temperature variations on FS
viscosity and predicted the water ux trends for the most appropriate
correlations between FO membrane and FS properties. The contribution
of water viscosity was investigated at different temperatures to the
water ux behavior; for comparison, the baseline experiment was
based on the entire FO and uPRO processes (Fig. 5a). The water ux
(Jw) behavior across the FO membrane can be expressed by Darcy's
law (Eq. (1)) [10]:
J w P= Rtotal

where P is the transmembrane pressure (Pa), is the absolute viscosity

of the permeate (kg m1 s1), and Rtotal is the total resistance of the
membrane (m1). The Jw values as a function of the solution temperature for both the FO and the uPRO process were positive, as shown in
Fig. 5a. Good agreement was observed between the experimental water
ux data and the solution viscosity inuence. The Jw values exhibited
generally constant trends with respect to the temperature variations; the
values of Jw were 2.42 0.34, 3.99 0.16, 2.65 0.24, 3.03 0.33,
2.56 0.47, and 6.81 0.43 109 mPa for 1 M NaClFO, 2 M NaClFO,

a
10
1 M NaCl-FO
2 M NaCl-FO
1 M KCl-FO
1 M CaCl2-FO
1 M Na2SO4-FO

2 M NaCl-PRO

-9

Jave * 10 m Pa)

4
2
0
0

10

20

30

40

50

Temperature ( C)

b
2.6

Resistance (*10

15

-1

m )

2.4
2.2
2.0

1 M NaCl-FO
2 M NaCl-FO
2 M NaCl-PRO
1 M KCl-FO
1 M CaCl2-FO
1 M Na2SO4-FO

1.8
1.6
1.4
1.2
1.0

Fig. 5. (a) Jave value with respect to the temperature and (b) membrane resistance at different DSs in the FO and uPRO modes. Operating conditions: pH = 6.5 and ionic
strength = 1 mM.

1 M KClFO, 1 M CaCl2FO, 1 M Na2SO4FO, and 2 M NaCluPRO DSs,

respectively.
Solution viscosities were calculated at different temperatures, which
were proportional to the membrane inherent resistances that are
shown in Fig. 5b. This phenomenon suggested that the water ux was
closely related to the solution viscosity, and that the solution viscosity is
a critical factor in the FO process at different temperatures. In addition,
the average water ux and water viscosity results suggested that the
membrane inherent resistance was not only greater in the FO mode
than in the uPRO mode, but also increased more in the presence of divalent solutes than in the presence of monovalent solutes, which is consistent with the results discussed above. Therefore, in real FO applications,
the operating temperature must be optimized to maximize the water
ux and ltration performance.
3.5. Inuence of solution temperature on reverse ux selectivity of the FO
process
We previously reported that both the type and concentration of the
salt inuence the ICP in narrow membrane pores and thus affect the
water ux and reverse solute ux performance. The reverse solute ux
typically increased linearly with increasing water ux, depending on
the membrane selectivity and the nature of the thermodynamic properties of the solutions. The RSFS is dened as the ratio of the water ux,
Jw, to the reverse solute ux, Js, in the FO process. We previously reported
that the RSFS is independent of the membrane SL properties and can
quantitatively describe the FO membrane performance according to
Eq. (2) [8,21]:
RSFS nA=BRT

where n is number of dissolved species created by the draw solute, T is

the absolute temperature of the solution (K), and R is the ideal gas constant (L bar K1 mol1).
As shown in Fig. 6a, the reverse solute ux increased as a function of
water ux regardless of different DSs. In the FO mode, increasing DS
temperature resulted in increasing water ux as a result of concentrative ICP, which was induced by the increase in the osmotic driving
force and reduction in the solution viscosity (Fig. 6b). Increasing the
DS temperature also resulted in an increase in the reverse solute ux,
which was caused by the elevated concentrative ICP of the draw solute
across the FO membrane SL. Fig. 6b also shows the dependence of the
membrane selectivity (the ratio of the water and solute permeability
coefcients deduced in the RO mode, as described in Fig. 1). Based on
the RSFS trends associated with the A/B coefcients in Eq. (2), the increase in the RSFS was higher in the presence of divalent salts (CaCl2
and Na2SO4) than in the presence of monovalent salts (NaCl and KCl).
This trend is inversely proportional to the solute permeability coefcients. The slopes of the RSFS curves as a function of solution temperature
in the FO mode were positive. The RSFS was expected to vary slightly
with the temperature (as suggested by Eq. (2)), since it is representative
of the ratio of the reverse solute ux to the water ux. The reverse solute
ux linearly increased with increasing water ux and induced lower
solution viscosities with increasing temperature. However, as shown in
Fig. 6b, increasing solution temperatures exerted greater inuence on increasing water ux than salt ux. This relative increase in the water ux
was attributed to the following phenomena: (i) The reductions in viscosity with increasing temperature were mainly attributable to hydrophilicity, which increased the wettability of the SL of the FO membrane; (ii)
during the FO process, less severe ICP decreased the resistivity to solute
diffusion within the SL, thereby enhancing the back diffusivity of the
draw solutes from the membrane AL and causing decreased permeation
of the draw solute towards the feed; and (iii) the temperature range
from 5 to 45 C in this study may have been sufciently wide to induce
changes in the membrane structural parameters; at higher temperatures,
a breakdown in thermally stable conditions may have led to the

Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012

J. Heo et al. / Desalination xxx (2015) xxxxxx

0.10

dominant factor during FO processes at different temperatures. Possible

changes in the membrane structural parameters occurred as the temperature ranged from 5 to 45 C; a breakdown in thermally stable conditions
and an improvement of water molecule diffusion kinetics rather than
solute diffusion resulted in an increase in the RSFS as a function of temperature. These results have signicant implications for the performance
of FO applications at elevated temperatures. Operating temperatures
must be optimized to maximize the water ux.

0.05

Acknowledgments

0.00

This research was supported by a grant (code 15IFIP-B088091-02)

from Industrial Facilities & Infrastructure Research Program funded by
Ministry of Land, Infrastructure and Transport of Korean government.

0.20
1 M NaCl
1 M KCl
1 M CaCl2

-2

-1

Reverse solute flux (mole m h )

0.15

1 M Na 2SO4
2 M NaCl

10

15

20
-2

25

-1

Ave. water flux (L m h )

Appendix A. Supplementary data

-1

Reverse flux selectivity (L mol )

Supplementary data to this article can be found online at http://dx.

doi.org/10.1016/j.desal.2015.06.012.

1 M NaCl
1 M KCl
1 M CaCl2

900
800

1 M Na 2SO4

References

2 M NaCl

700
600
200
150
100
50
0

10

20

30

40

50

Temperature ( C)
Fig. 6. (a) Reverse solute ux as a function of average water ux and (b) reverse ux selectivity at various temperatures in the FO mode with different DSs. Operating conditions:
pH = 6.5 and ionic strength = 1 mM.

improvement of water molecule diffusion kinetics rather than solute

diffusion, thereby leading to a greater increase in the water ux compared with the salt ux [25]. In summary, higher temperatures led to
an increase in the RSFS, not only via greater reduction of CP resistances
of FO membrane (AL as well as SL), but also via increasing the wettability
within the effective porosity of the SL.
4. Conclusions
The water ux and fouling propensity of several DSs (based on KCl,
NaCl, CaCl2, and Na2SO4) were evaluated to systematically investigate
the temperature inuence on available FO membranes in FO and
uPRO processes. The RSFS at different temperatures was also evaluated
to characterize the transport mechanisms. The membrane selectivity
(A/B) based on the SD model approach followed the order KCl N
NaCl N CaCl2 N Na2SO4. The higher solute permeabilities of NaCl and
KCl were attributed to the smaller hydration radii of Na+ and Cl compared to those of Ca2+ and SO2
4 . The temperature signicantly inuenced the magnitude of the water ux in the FO mode, since increasing
temperature greatly reduced the ICP across the membrane, thereby
resulting in changes in the thermodynamic properties, such as osmotic
pressure, diffusion coefcient, and viscosity of the FSs and DSs. Signicant
ux reduction was observed after SA was introduced into the FS at low
temperatures. The ux reduction was attributed to the synergistic interactions between the solution viscosity and the formation of a more
dense cake layer on the membrane surface. The osmotic pressures of
the divalent DSs were inversely proportional to their solute diffusivities,
since the inuence of ICP was greater for the larger, divalent ions. The
water ux was closely related to the solution viscosity and was a

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Please cite this article as: J. Heo, et al., Organic fouling and reverse solute selectivity in forward osmosis: Role of working temperature and
inorganic draw solutions, Desalination (2015), http://dx.doi.org/10.1016/j.desal.2015.06.012