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Performance Evaluation of Aquaporin Forward Osmosis Membrane Using Chemical
Performance Evaluation of Aquaporin Forward Osmosis Membrane Using Chemical
Mirshekar J.L1, Kamarehie B1*, Jafari A1, Ghaderpoori M1, Karami MA1, Sahebi S2, 3*
1
Department of Environmental Health Engineering, Faculty of Health and Nutrition, Lorestan University of Medical Science
Khorramabad, Iran
2
Environmental Engineering and Management Research Group, Ton Duc Thang University, Ho Chi Minh City, Vietnam
3
Faculty of Environment and Labour Safety., Ton Duc Thang University, Ho Chi Minh City, Vietnam
*
Corresponding Authors: Email: b.kamarehie@lums.ac.ir (B. Kamarehie) and Soleyman Sahebi:
E-mail: soleyman.sahebi@tdtu.edu.vn
Abstract
osmosis (FO) membrane was evaluated with several commonly used fertilizers ((CO (NH2)2,
KCl, CaCl2, (NH4)2SO4 and (NH4)2HPO4) as a draw solutions (DSs) to verifying the possible
implementation of this AQP-FO membrane in the fertigation industry. Also, DS and feed
solution (FS) concentrations were evaluated under FO and pressure retarded osmosis (PRO)
operation modes. The results showed that CaCl2 seems to be a more suitable DS in terms of the
tradeoff between water flux and salt permeability, compared to the other DSs used in this study.
However, KCl gained the highest performance in terms of water flux which was 13.9 Lm-2 h-1
and 24.1 Lm-2 h-1 in the FO and PRO mode, respectively. The performance of the AQP
membrane in terms of water flux and reverse solute flux can be improved by modifying the
This article has been accepted for publication and undergone full peer review but has not been
through the copyediting, typesetting, pagination and proofreading process which may lead to
differences between this version and the Version of Record. Please cite this article as doi:
10.1002/ep.13536
Increasing demands for freshwater along with a high standard of living and development in
industrial and agricultural sectors would make water a more important commodity even more
than oil in the near future [1]. According to World-watch Institute, by 2025, over two-thirds of
the earth's population will face water shortage which will put mankind's survival at risk [2].
Different desalination and wastewater reclamation methods have been developed during the last
century [3]. The state of the art of the Reverse Osmosis (RO) desalination process has dominated
the desalination technology. However, high energy consumption in this pressure driven
technology, membrane fouling, and brine discharge remain the main obstacles for the RO
process [4, 5]. Recently, researchers have paid more attention to newly emerged technology,
Forward Osmosis (FO), which requires much less energy with sensible advantages and can be
FO requires no hydraulic pressure, is less prone to fouling, and more environmentally friendly
This process occurs spontaneously like natural osmosis as osmotic agents generate osmotic
pressure which pulls water molecules from a side of a low concentrated solution across a semi-
permeable membrane [12, 13]. Generally, in the FO process, DSs are required to be separated
and recovered in an additional step when the main objective of the FO desalination process is to
produce potable water [13]. Thus, this may require energy. Nevertheless, an appropriate osmotic
the DS recovery is not needed [14, 15]. For example, DS separation in the FO process for
agricultural purposes is not required when chemical fertilizers are used as DS [16, 17]. Diluted
DS can be used directly in the farm and by this, water and nutrients can be available together for
Typically, membranes used in FO are made of Cellulose Triacetate (CTA) or Thin Film
Composite (TFC), which makes the situation easy for water to cross the membrane from FS side
to DS side; however, these membranes reject organic matter and ions to permeate [20-23]. TFC
membranes as a new FO membrane type are widely used for FO applications in different
industries. For example, the FO process could be an alternative separation process for oily [24],
and radioactive wastewaters [25, 26]. Studies have reported that TFC due to high selective
polarization, leading to less water flux [29]. Therefore, researchers are attempting to make use of
new and better membranes with high mechanical and chemical resistance to provide higher water
flux and saline compounds rejection and to minimize Internal Concentration Polarization (ICP)
[22, 30-33].
Taking inspiration from nature and in order to provide high water flux with the aid of natural
that act as channels to transfer water across cell membranes. Under the right and real conditions,
these proteins form water channels, which can exclude and reject salt ions while permeating
water molecules. Unique properties of AQPs with water permeability and salt rejection (SR)
have recently received much interest to apply as infrastructure for biomimetic membranes for
The first attempt to fabricate an AQPs incorporated membrane were focused on strategies that
include fixing proteins on a template as free-standing polymer films or lipid [36, 37]. Kumar et
al. 2007, developed the first biomimetic membrane for the FO process by bursting AqpZ-
on, Tang research group used conventional interfacial polymerization method for making the
AQPs-FO membrane which opened a scalable approach to making the AQPs-FO membrane on a
roll-to-roll basis on an industrial scale [39, 40]. The capability of the commercial AQPs-FO
membrane had been evaluated for the removal of heavy metals in industrial wastewater [41].
This study aims to investigate the performance of newly commercialized AQP membranes in the
FO process using commonly used fertilizers. This is the first study on evaluating five commonly
used fertilizers as DS for desalination of feed water with different TDS for AQP FO membrane.
Water flux and Reverse Solute Flux (RSF) for FO and Pressure Retarded Osmosis (PRO) modes
were carefully investigated. The post-treatment process and volume of water required for further
presented in this work as it has been investigated in earlier studies [19, 42].
2. EXPERIMENTAL
Five different chemical fertilizers typically applied for agricultural purposes including,
((NH2)2CO, KCl, CaCl2, (NH4)2SO4, (NH4)2HPO4 were used as concentrated DS. All materials
used in this study were of analytical grade and provided from (SAMCHUN, Korea). Four
dissolving the chemical fertilizers in deionized water. Deionized water (DI) and NaCl in
concentrations of 5-35 g/l was used as FS. NaCl solution with different concentration levels was
used as brackish and seawater, indicating the FS total dissolved solids (TDS).
The FO membrane used in this study was AQP-based (Aquaporin Asia Pte. Ltd, Singapore)
membranes. The rejection capacity of the membranes was > 99.0% ± 0.5 % according to the
company’s report for Calcein. The membrane cross-section and top surface morphologies were
studied using a high-resolution Schottky Field Emission Scanning Electron Microscope (FE-
SEM, MIRA3-LMU model, Czech Republic, Million times magnification). For this purpose,
membrane substrates were first dried carefully at room temperature for 24 h. The samples were
cracked by immersing in liquid nitrogen and thereafter coated with thin layers of gold using
Balzers Sputter coater (SCD 050, BAL-TEC, Germany) before SEM imaging.
Membrane porosity (ε) was also measured by weighing the wet mass (W1) and the dry mass (W2)
(𝑊𝑊𝑊𝑊 − 𝑊𝑊𝑊𝑊)/𝜌𝜌𝜌𝜌
𝜀𝜀 = × 100%
𝑊𝑊𝑊𝑊 − 𝑊𝑊𝑊𝑊
� 𝜌𝜌𝜌𝜌 � + [𝑊𝑊𝑊𝑊/𝜌𝜌𝜌𝜌]
(1)
where is the density of the wetting solvent and is the density of the membrane.
The SR (Rs) and water permeability coefficient (A) of the Biomimetic-FO membrane were
determined based on the pure water fluxes obtained in the RO mode using the same membrane
cell at different pressures ranging from 0 to 5 bar. SR property of the Biomimetic-FO membrane
was determined by measuring the electrical conductivity of the feed (1000 mg/L NaCl) and the
permeate water at 5 bar applied pressure. The salt permeability coefficient (B) was then
1− R B
= (2)
R A(∆P − ∆π )
Where Δπ is the net osmotic pressure difference between the feed and the permeate and ΔP is the
The membranes were examined in both FO (active layer in contact with the FS and supported
layer with concentrated DS) and PRO modes vice versa. A lab-scale FO process cell similar to
sides, providing a useful area of 6.2 cm2. The experiments were made in a batch mode in which
flows of FS and DS were maintained at 400 ml/min. A two-way pump (Pumpdrive 5001,
Heidolph-Germany) was applied to recirculate feed and DS through both sides of the membrane.
Each experiment was set for 30 min with an equal initial volume of 250 ml for FS and DS.
Figure 1 shows the schematic of the lab-scale experimental setup for the FO process.
Performance of the membrane was analyzed in terms of water flux (Jw), reverse solute flux
(RSF), and specific reverse solute flux (SRSF). Water flux (Jw) was measured immediately via
connection of the concentrated DS container to scale and computer. Water flux (Jw) was
calculated from the changes in the weight of the DS during each run of the experiment,
expressed as follows:
∆m / ρ w (3)
Jw =
Am .∆t
where JW is water flux (L/m2h), is the weight difference of DS as it increases during the time
of each run of the experiment (g), denotes the useful membrane area (m2), is the time of
Once deionized water was considered as feed water, RSF was measured using a multimeter
(Lutron-CD4303, Germany) to measure electrical conductivity (EC) of the FS at the end of each
formula:
∆(CtVt )
Js = (4)
Am ∆t
where Vt and Ct are feed solution volume and salt concentration, respectively. Am and Δt are
active membrane surface and experiment time. Reverse solute flux (Js) is expressed as g/m2h.
<Figure 1>
Fig. 2 shows the SEM images of the AQPs membrane substrate for the cross-section, membrane
top, and back surface. Fig. 2(a) shows the AQPs membrane top surface. It is interesting to see
that AQPs membrane rejection layer which is formed by AQPs proteins is similar to thin film
composite membrane polyamide layer in terms of topology [31]. This AQPs-FO membrane is
developed by aquaporin incorporation into the polyamide layer during interfacial polymerization.
Fig. 2(b) also shows the back surface of this membrane with non-woven backing fabric support.
The commercial TFC FO and CTA FO membrane have woven polyester mesh backing fabric
and SEM images can be found in other studies [44]. Fig. 2(c) shows the membrane cross-section
which contains a large number of finger-like pore structures, which produce relatively higher
choosing the right polymer concentration and solvent/non-solvent during phase inversion [22].
Table 1 also shows other membrane characteristics. The contact angle of AQPs membrane top
surface has a contact angle of 45°, while the contact angle for the bottom surface, which is non-
woven backing fabric is 75°. Relatively lower contact angle in the top surface may be related to
the proteins and lipids created water channels; the increased hydrophilicity is a desirable factor
<Figure 2>
<Table 1>
A recent study showed by CFD modeling that the porosity (support layer) has an effect on both
RSF and forward water flux. Considering this, increasing support layer porosity or reducing
tortuosity within is not always and necessarily desirable since it may also result in higher RSF
[45].
The A, R, and B values of the AQP FO membrane were determined in the cross-flow RO
operation as described earlier (Table. 2). Pure water permeability was determined using DI water
as the feed in RO mode at applied pressures ranging from 0 to 5 bars. R was tested using
High water permeability can be achieved while R sacrificed and this can be vice versa as well.
This means by having tighter and well-formed rejection layer, R substantially improved with
membrane for the FO process which relates to the different nature of the rejection layer in
biomimetic embedded into polyamide membrane compare to the conventional polyamide layer
<Table 2>
The membrane performance was tested in terms of water flux in the FO mode with different DS
concentrations while DI water was used as FS. (NH4)2SO4, KCl, CaCl2, (NH4)2HPO4 and
(NH2)2CO (Urea) fertilizers were selected as DSs (Standard error bars are applied). Fig. 3 shows
the performance of 5 different DS as obtained water flux using DI water in the FO process were
KCl with 18.019 Lm-2 h-1 and urea with 7.381 Lm-2 h-1 at concentration of 3 M were recognized,
respectively to be with the highest and lowest flux among 5 different solutions. In a study
conducted on the TFC membrane, a flux of 27.89 Lm-2 h-1 was reported when KCl 1M and DI
water were considered as DS and FS [46], respectively, which is significantly higher than that of
Regarding the low performance of urea, it is a natural compound and generates much lower
osmotic pressure at a similar molar concentration compared to monovalent fertilizer such as KCl
or divalent compounds such as CaCl2 (monovalent anion and divalent cation). Prediction made
55 (atm) while for CaCl2 with similar molar concentration is 342 (atm) [46]. Furthermore,
another reason for low water flux for urea can be attributed to the hydrophobic characteristic
which plays an important role to limit the connection between urea and support layer of the
membrane [17, 46]. Therefore, it is noteworthy that the type of DS is a crucial factor in the FO
process for fertigation. Also as shown in Fig. 2, at higher concentration levels of DS, the pure
osmosis pressure as the main factor for passing water cross membrane is higher. Therefore,
Fig. 4 shows the results of water flux performance in FO and PRO modes for all DSs at 1 M
concentration (Standard error bars are applied). As can be seen from Fig.4, the amount of water
that passed through the membrane in PRO mode is considerably higher than that of FO
condition, which is in line with other documented studies [46-49]. This is due to less ICP in PRO
mode and having higher osmotic pressure thanks to the higher concentration level of DS on the
membrane surface close to the active layer, which can generate more driving force and finally
porous support layer and FS in touch with membrane active layer, the water flux passing through
FS dilutes the DS on the membrane surface and the porous support layer, which finally reduce
the osmotic pressure and water flux. Given that the osmotic pressure of DS on the active layer is
more important and is a determining factor for the FO process, the water flux can be extremely
influenced by dilutive ICP [22]. The inverse CP can occur when the process is in PRO mode,
concentrated ICP occurs in the side of FS, the effect of this function is less compared to dilutive
ICP, as the water flux in PRO state is accordingly higher than FO mode [49].
PRO condition, although in lab-scale experiments and under controlled conditions generates
more water flux, but in reality, as the porous support layer of the membrane is more prone to
scaling elements, the membrane is subjected to more fouling and this state is not applicable for
water desalination [46]. This is especially important in the FO process for fertigation where
blended fertilizer as DSs was used. Although sever membrane scaling was not observed in this
study, however, using a blend of conventional fertilizer for farming as DS can potentially contain
several monovalent and divalent ions. This can increase the chance of physical scaling by
reacting with the RSF ions coming from the FS side [50].
<Figure 3>
<Figure 4>
For evaluating the further role of PRO mode, KCl as the best fertilizer in terms of water flux
performance was chosen to be tested under both FO and PRO modes at different molar
concentrations. Fig. 5. Shows, although higher flux increases by increasing the molar
concentration of DS, this trend doesn’t follow a linear correlation, meaning increases in DS
concentration will not necessarily increase the proportionally estimated water flux (Standard
error bars are applied). Non-linear correlation between water flux and DS concentration indicates
which are in agreement with other similar studies [46, 47, 51].
Figs. 6 and 7 represent the performance of membrane for the FO process in terms of reverse
solute flux (RSF) and specific reverse solute flow (SRSF), respectively (Standard error bars are
applied). The ranked performance of 5 different DS for the FO process in terms of RSF was:
Urea>KCl>(NH4)2SO4>(NH4)2HPO4>CaCl2. The highest RSF was found for urea (31.462 gm-2h-
1
in the concentration of 3 M) and the lowest was CaCl2 (6.210 gm-2h-1 in the concentration of
3M). The amount of RSF depends on the type of solute, the value of hydrated ions, membrane
structure, and operating parameters such as temperature and water flux [52]. Lower RSF is
<Figure 6>
<Figure 7>
As shown in Fig. 6, urea as DS causes the highest amount of wasting solute through RSF among
the 5 different DS used in the present study. The high RSF of urea can be attributed to low
inhibition of urea through the membrane because urea has the lowest molecular size compared to
other types of DS used in this study. Following urea, the highest RSF can be regarded as KCl.
When compared with bivalent compounds, KCl as a monovalent is likely to have a lower
inhibition rate [16, 17, 53]. (NH4)2SO4 and (NH4)2HPO4 with monovalent cations and bivalent
divalent cation and monovalent anion in its chemical structure, which limits its reverse solute
flow through the membrane active layer. The RSF plays an important role in the economic
assessment of the FO process because the less reverse solute reduces the wasting amount of DS.
The ratio of reverse solute flux to water flux passing through a membrane is recognized as a
specific reverse solute flux (SRSF). Fig. 7 shows SRSF of DS at different concentrations using
DI water as FS in the FO mode. SRSF can show the membrane selectivity regardless of the
concentration of DS. SRSF along with two other parameters of water flux and salt inhibition are
used for the assessment of membrane performance in the FO process. The lesser the SRSF value,
the higher the efficiency and selectivity of the membrane that will be achieved [3]. According to
the results presented in Fig. 6, RSF increases with the concentration levels of DS for all
experimented DS. This is because the high concentration levels of DS cause more differences of
reverse osmotic pressure, which make ions to extremely return to FS. In other words, by
reduction of DS concentration and driving force which occur in series, RSF is decreased [53].
However, SRSF almost stays constant irrespective of the increase in DS molar concentration as it
In the present study, 2 different concentration levels of NaCl were used for FS to stimulate the
brackish and seawater. Different concentration levels of 5 g/L and 35 g/L NaCl (BW 5, BW35)
were prepared in terms of TDS in water. The TDS concentration levels of FS can directly affect
shown in Fig. 8. The performance and efficiency of 5 different DS in terms of water flux and
feed) is slightly different compared to DI water used as a feed. CaCl2 showed better performance
in comparison with (NH4)2SO4 when BW water was used as feed. While most fertilizers
containing monovalent ions did not result in any scaling when used as an FO draw solution (DS),
fertilizer with divalent ions resulted in scaling due to RSF interaction with ions in the feed
solution. A previous study by Sherub et al. confirmed that fertilizers with divalent ions such as
(NH4)2HPO4 caused significant scaling, which contributed to flux decline and poor performance
[50]. CaCl2 is recognized as the second DS with high water flux after KCl. The high solubility
and osmotic pressure are considered as two distinct properties of an appropriate DS [3]. The type
of DS and its osmotic pressure together affect considerably the performance of the membrane in
the FO process [46]. Achili et al. studied the performance of DS from the perspective of
NaHCO3 and concluded that of these DS, CaCl2 had the highest efficiency [53].
When BW5 was used as FS, KCl (15.990 LMH at a concentration of 3 M) and urea (5.223 LMH
at a concentration of 3M) were found to DS with the highest and lowest water flux, respectively.
NaCl 5 g/L as FS for the FO process, and water flux of 18.95 LMH was reported [46].
The results revealed that when BW was used as FS, concentrated ECP which occurred on the
side of the active layer reduced the effective driving force more than DI and finally minimizes
the water flux. Therefore, it can be considered as a point of reducing the water flux when BW is
applied as DS compared to DI. The results obtained in the present study favor other similar
At a constant concentration level of DS, increases in TDS of FS cause reduction of pure osmotic
pressure and subsequently, reduction in water flux. Indeed, these results indicate that the effect
of the degree of concentrated ECP on FS increases when FS of high TDS is used. It is assumed
that this increase can result from increases in the viscosity of FS with high TDS, which decreases
Fig. 9 shows the comparison of the water flux of the same five fertilizers as a DS at different
Similar to the RO process, FS concentration has a major role in the performance of the FO
process as the osmotic pressure of the FS can affect the driving force or net osmotic pressure.
Comparing Figs. 8 and 9, the water flux decreased with the increase in feed TDS in all DS level
of Molar concentrations due to a decrease in the net osmotic pressure caused by high FD TDS
(Standard error bars are applied). For example, at the 3 molar DS concentration in Fig. 8 where
the with BW5 as FS, water flux of 16.1 Lm-2h-1 was achieved for KCl, however, Performance for
BW35 resembling seawater was used. Thus, increasing FS TDS can reduce the net driving force
more important. Thus, brackish water or wastewater is more attractive for fertigation as seawater
<Figure 8>
<Figure 9>
4. Conclusions
Based on the results, CaCl2 had better performance on average when compared with other DSs
evaluated in this study, which refers to its chemical characteristics and/or generating more
osmotic pressure as a driving force. In the PRO mode of operation, the net gain water flux was
more compared to the FO condition which shows more severe effect of ICP in the FO mode of
operation. Although it seems that the water flux produced from this membrane is lower
compared to other typically applied membranes with polyamide inhibitive layer for the FO
process, however, this may be a step in the right direction to bring natural transporters such as
aquaporins to membrane industries. Further research on the AQP-based membrane with regard to
fouling to know more about the characteristics of the membrane to be applied in the specific
This study is supported by Lorestan University of Medical Science. The authors are deeply
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Table 1.
Thickness
Sample ID Porosity% Contact angle (º)
(µm)
Table 2.
a c
Sample ID Water permeability (A) b
Salt permeability B NaCl rejection (%) S value
a
Evaluated in the RO testing mode over an applied pressure of 5 bar with DI water as feed water.
b
Evaluated in the RO testing mode over an applied pressure of 5 bar for feed water containing 1000 mg/L NaCl.
c
Evaluated based on experiments under the FO mode using 2 M NaCl as the DS with DI water as feed water.
Figure 2. SEM image of the AQP membrane displaying (a) the top surface of the active layer (b) the bottom
surface and (c) the cross-section of the membrane.
Figure 3. Comparison of water flux for DS at different M concentrations using DI water as a FS in the FO
mode of operation.
Figure 4. Comparing water flux in FO and PRO mode using DI water as FS and for DSs at 1 M concentration.
Figure 5. Comparing water flux in FO and PRO mode using DI water as FS at different M concentration for
KCl.
Figure 8. Comparison the water flux of different fertilizers as a DS at different concentrations using 5000
mg/L NaCl as FS in FO mode.
Figure 9. Comparison the water flux of different fertilizers as a DS at different concentrations using 35000
mg/L NaCl as FS in FO mode.