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Evaluation of food additive sodium phytate as a novel draw solute for forward
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DOI: 10.1016/j.desal.2018.10.004

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 Desalination 448 (2018) 87–92

Contents lists available at ScienceDirect

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

Evaluation of food additive sodium phytate as a novel draw solute for T

forward osmosis
⁎
Jiaqi Huanga,b,c,1, Shu Xionga,b,c,1, Qingwu Longd, Liang Shena,b,c, Yan Wanga,b,c,
a
Key Laboratory of Material Chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology), Ministry of Education, Wuhan, 430074, PR
China
b
Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science & Technology, Wuhan,
430074, PR China
c
Shenzhen Institute of Huazhong University of Science and Technology, Shenzhen 518000, PR China
d
School of Chemistry and Chemical Engineering, Lingnan Normal University, Zhanjiang 524048, PR China

G R A P H I C A L A B S T R A C T

A R T I C LE I N FO A B S T R A C T

Keywords: Proper draw solution is a crucial factor to generate a high performance in FO process. In this study, a phytic acid
Forward osmosis and its salt (PA-Na) were evaluated as novel draw solutes in FO process. The effects of the solution pH and
Draw solution concentration on the physicochemical properties were investigated systematically. Using 0.45 M PA-Na draw
Phytic acid salt solution (pH = 7) and DI water feed solution, a relative high water flux of 19.02 LMH and a low solute flux of
Food additive
0.51 gMH can be obtained, with HTI-TFC membrane in the PRO mode. An even better performance of a
Brackish water desalination
30.35 LMH water flux and a 0.61 gMH solute flux can be achieved using the self-made HPAN-TFC membrane.
The comparison of PA-Na and NaCl draw solutions shows that PA-Na draw solution has a much lower draw
solute leakage and a competitive water flux. In addition, the application of PA-Na draw solution for the brackish
water desalination was explored. The diluted PA-Na draw solution after FO may be used directly in food pro-
duction by further dilution. In general, the non-toxicity and satisfactory FO performance of this food additive
demonstrate its great potential as a draw solute for FO applications.

⁎
Corresponding author at: Key Laboratory of Material Chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology), Ministry of
Education, Wuhan 430074, PR China.
E-mail address: wangyan@hust.edu.cn (Y. Wang).
1
The first two authors contribute equally to this study.

https://doi.org/10.1016/j.desal.2018.10.004
Received 8 February 2018; Received in revised form 21 September 2018; Accepted 1 October 2018
Available online 06 October 2018
0011-9164/ © 2018 Elsevier B.V. All rights reserved.
J. Huang et al. Desalination 448 (2018) 87–92

1. Introduction
O
Forward osmosis (FO) is a membrane-based technology driven by
the osmotic pressure between the feed solution and the draw solution
HO P
[1–5]. Compared to traditional reverse osmosis and nanofiltration O
driven by external hydraulic pressure, FO has a lower energy require-
HO O
ment and exhibits a reduced membrane-fouling tendency [6–9]. Thus,
OH P OH
FO has attracted increasing research interest in recent years and ex-
O
hibited great potential for various applications in desalination, water P
treatment, power generation, and so on [10–14]. O OH
Draw solutions play a critical role as osmotic pressure suppliers; HO O
regardless, research about draw solutions relatively lags behind [15]
because of prerequisites that have to be fulfilled, including the fol- O
lowing: (1) a high osmotic pressure to generate a high water flux; (2) a O
suitable molecular size to ensure low reverse draw solute leakage; (3)
convenient recovery at a low cost; (4) nontoxicity; and so on [16]. P O O P
Commonly used draw solutes include inorganic salts such as sodium
HO
chloride (NaCl) and magnesium chloride (MgCl2) [17,18]. These salts
O HO OH
can be ionized completely and generate high osmotic pressure in the OH
aqueous solution, ensuring considerably high water fluxes in FO; OH
however, salt leakage is also extremely severe and entails high energy
consumption in the draw solution recovery. Magnetic nanoparticles, HO P
thermosensitive polyelectrolytes, and thermally responsive hydrogels
have been developed as potential draw solutes [19,20] with negligible O
solute leakage and easy recovery. However, they generally exhibit low
water fluxes. As draw solutes, thermolytic salts [10,21,22], such as Fig. 1. Chemical structure of phytic acid.
ammonium bicarbonate (NH4HCO3), can produce high water fluxes in
FO and be easily recovered by decomposition with industrial waste hydroxide (NaOH) (≥96%) were acquired from Sino-pharm Chemical
heat. However, the corrosive and harmful nature of ammonia gas (NH3) Reagent Co. (Shanghai, China). Deionized water (DI water) with a re-
may deteriorate the quality of the product water with even a slight sistivity of 18.25 MΩ·cm was generated from Wuhan Pin Guan
residue of the draw solute. Various organic acid salts were subsequently Ultrapure Water LAB System (China).
developed as potential draw solutes with superior FO performances
because of their ionogenic chemical structures in the aqueous solution 2.2. Preparation of PA-Na draw solution
and suitable molecular size, which can ensure high water flux, low
viscosity, and relative ease in draw solution recovery [23–28]. PA-Na draw solutions of different pH values were prepared by di-
Draw solutes based on natural compounds present advantages over luting the PA aqueous solution with the designed concentration and
other compounds because draw solutes cannot be used to obtain po- adjusting the pH with NaOH, where the solution pH was determined
table water directly without a regeneration step. For instance, a “draw with a pH meter (Mettler toledo, FE28).
water” bag with edible products as the draw solute can obtain water
from contaminated water in the wilderness [29]. Nontoxic gluconate 2.3. Osmotic pressure and relative viscosity of PA-Na solution
salts have also been reported as novel FO draw solutes with good FO
performance for the reconcentration of various fruit juices [29]. Simi- The osmotic pressures of PA-Na aqueous solutions were measured
larly, sodium lignin sulfonate and commercial fertilizers reported as FO using a home-made lab-scale setup [23] based on the freezing point
draw solutes can also be directly applied in crop irrigation after dilution depression method and calculated by Eq. (1):
via FO [30,31].
T0 − Tt
In the present study, phytic acid (PA) and its sodium salt (sodium π= × 22.66
1.86 (1)
phytate, PA-Na), which are natural green additives used in the food and
pharmaceutical industries [32–35], are explored as draw solutes for where T0 and Tt are the freezing points of DI water and the PA-Na so-
applications in FO for the first time. Fig. 1 shows the chemical structure lution respectively.
of phytic acid. Numerous phosphate groups are found in the molecule, The determination of relative viscosities (ηr) of PA-Na aqueous so-
which can easily ionize and produce high osmotic pressure in the lutions was conducted with a commercial Ubbelohde viscometer at
aqueous solution. The molecular weight of PA is 660, which can suf- 25 ± 1 °C and calculated with Eq. (2):
ficiently ensure low-solute leakage in FO. In addition, both PA and PA- η ρt
Na are environment- and human-friendly [32]. These advantages of PA ηr = =
η0 ρ0 t 0 (2)
suggest its potential as a desirable draw solute. In the current study, the
effects of both the pH and concentration of the PA solutions on FO where t0 and t (s) are the outflow time of the DI water and PA-Na so-
performance are systematically evaluated. The PA-Na draw solution is lution, respectively, ρ0 and ρ (g/cm3) are the densities of DI water and
further evaluated for brackish water desalination by FO. This study can PA-Na solution detected by a density meter (KEM DA-130 N, Japan).
potentially contribute to the development of new draw solutes for FO.
2.4. FO process
2. Materials and methods
FO tests were carried out by a commercial lab-scale FO faclity
2.1. Materials (Suzhou Faith Hope Membrane Technology) with a fixed effective
membrane area of 3.87 cm2. Two kinds of FO membranes were used to
Phytic acid (PA) (70% aqueous solution) was supplied by Aladdin evaluate the FO performance of PA-Na draw solution, i.e., the com-
(Shanghai, China). Sodium chloride (NaCl, ≥99.5%). Sodium mercial thin film composite (TFC) FO membrane from HTI (Hydration

88
J. Huang et al. Desalination 448 (2018) 87–92

Table 1 20 2.25
Basic FO performance of HTI-TFC and self-made HPAN-TFC membranes. Osmotic pressure

Osmotic pressure (bar)

Membrane Water flux (LMH) Salt leakage Membrane orientation 19 Relative viscosity

Relative viscosity
note (gMH)

HTI-TFC 7.13 ± 0.22 5.13 ± 0.18 PRO mode 18 2.00

3.98 ± 0.13 2.75 ± 0.15 FO mode
HPAN-TFC 17.16 ± 0.73 9.29 ± 0.68 PRO mode 17
9.72 ± 0.82 4.99 ± 0.35 FO mode

Note: DI water and 0.5 M NaCl solution were used as the feed solution and draw 16 1.75
solution respectively.
15
Technologies Inc., OR, USA) (HTI-TFC) and the homemade TFC mem-
brane prepared by interfacial polymerization of m-phenylenediamine 14 1.50
and trimesoyl chloride on the surface of the hydrolyzed poly- 6 7 8 9
acrylonitrile substrate (HPAN-TFC), as characterized in our earlier work
[36]. The details about the membrane fabrication can be found in the pH
Supporting information. FO performance with HTI-TFC and self-made
Fig. 2. The osmotic pressure and relative viscosity of PA-Na solutions with
HPAN-TFC FO membranes was evaluated and shown in Table 1, using
different pH (0.15 M).
0.5 M NaCl solution as the draw solution and DI water as the feed so-
lution. During the FO test, both feed and draw solutions were looped at
the same volumetric flow rate (300 mL/min) at room temperature draw solution was shown in Fig. S2 in the Supporting Information.
(25 ± 1 °C). FO performance in both FO mode (feed solution facing the
selective layer) and PRO mode (draw solution facing the selective layer)
3. Results and discussion
was tested. The water flux (Jw, L/m2·h, referenced to as LMH) was
calculated by Eq. (3):
3.1. PH optimization of PA-Na solution
∆m
Jw =
A × ∆t × ρ0 (3) PH optimization of PA-Na solution was conducted to achieve the
desired FO performance. To prevent the impairment to the TFC mem-
where Δm (g) is the weight increase of the draw solution during a
brane, a relative neutral pH range (6–9) for the draw solution was used
predetermined time Δt (h), A (m2) is the effective membrane area.
in this study. As shown in Fig. 2, the osmotic pressure of the PA-Na
The reverse solute flux Js (g/m2·h, noted as gMH) was obtained
solution increases with an increase in solution pH. Such rise in osmotic
according to Eq. (4):
pressure could be attributed to the generation of more ions in the
(Ct V)
t − (C 0 V0 ) aqueous solution when phosphoric acid groups in phytic acid are con-
Js =
A × ∆t (4) verted to sodium phosphate groups, which is similar with results ob-
where C0 and V0 are the initial concentration and feed volume of the tained in previous reports [24]. This hypothesis is verified by the
feed solution, while Ct and Vt are the concentration and the feed volume conductivity measurements of the four draw solutions, which are listed
after a predetermined time Δt. The feed concentration can be measured in Table 2. The conductivities obey the order of osmotic pressures [18].
using a calibrated conductivity meter (Mettler toledo, FE30). Calibra- With an increase in pH by adding NaOH, neutralization occurs to
tion curves of the solution conductivity vs PA-Na concentration with convert eH2PO3 groups to eHPO3−Na or ePO32Na groups, which are
different solution pH were shown in Fig. S1 in the Supporting In- dissociated more easily in the aqueous solution. A higher conductivity
formation. indicates the generation of a larger number of free ions in PA-Na so-
lution and enhanced dissociation of PA-Na with the increase in pH, and
2.5. Application of PA-Na in FO process consequently, a higher osmotic pressure. Fig. 2 also shows that relative
viscosity increases with an increase in solution pH because of increased
The potential of PA-Na draw solution for the brackish water treat- mass concentration with the addition of NaOH into the solution.
ment was further investigated with 0.15 M NaCl aqueous solution as Consequently, the FO flux increases when the pH of the PA-Na so-
brackish water feed solution and 0.45 M PA-Na solution as the draw lution increases, as shown in Fig. 3, which is attributed to the increased
solution for a 30-min FO test. The test conditions were the same as osmotic pressure. However, the increase in water flux does not exhibit
those described in Section 2.4. the same linear trend as that of the osmotic pressure. The difference
could be attributed to the increased severity of the internal con-
centration polarization (ICP) arising from the higher viscosity of the PA-
2.6. NF recovery of draw solution
Na solution at a higher pH [37]. Simultaneously, the solute leakage of
the PA-Na solution also increases with an increase in pH because of a
The draw solution recovery after the FO test was also studied by a
rise in the number of ions (Na+) generated in the solution. Because Na+
pressure-driven NF process (Cross-flow NF setup, Suzhou Faith Hope
ions are easier to leak through the membrane owing to its much smaller
Membrane Technology) under a 2 bar upstream pressure with a com-
size than PA anions and the electrolytic attraction with the negatively-
mercial flat-sheet NFW membrane (Snyder Filtration, with an effective
charged membrane surfaces [38,39], more Na+ ions in the draw solu-
membrane area of 7.065 cm2 and MWCO of 300–500 Da). The water
tion could result in a higher reverse draw solute leakage. Accordingly,
permeability and the salt rejection (R) were evaluated by Eqs. (3) and
(5) respectively.
Table 2
C The conductivity of various draw solutions (0.15 M) at 25 °C.
R = ⎛1 − P ⎞ × 100%
⎜ ⎟

⎝ Cf ⎠ (5) pH 6 7 8 9

where Cp and Cf (mg/L) are the concentrations of the permeate and feed Conductivity (ms/cm) 41.7 42.5 43.2 44.1
solutions, respectively. The recovery performance of diluted PA-Na

89
J. Huang et al.
Fig. 3. The effect of draw solution pH on the FO performance (feed solution: DI
water, PRO mode).
the specific reverse solute flux (Js/Jw) fluctuates with an increase in pH,
with the lowest value (0.037) obtained at pH = 7. The Js/Jw value,
which is generally used to reflect the loss of the draw solute per unit
volume of the water permeation in FO, is a significant index reflecting
the efficiency of the draw solute [40]. Notably, the Js/Jw value of the
PA-Na draw solutes ranges from 0.037 g/L to 0.056 g/L, which is con-
siderably lower than that of a typical NaCl draw solution (0.4–1.14 g/
L), indicating the high potential of this proposed PA-Na draw solute.
3.2. Effect of PA-Na concentration
The concentration of the draw solution is an important factor in-
fluencing FO performance. Draw solutions of a higher concentration
can generally produce a higher osmotic pressure and a corresponding
higher water flux in FO. However, the higher solution concentration
may lead to a higher viscosity of the draw solution, increasing the se-
verity of internal concentration polarization (ICP) and ultimately
leading to a water flux decline [41,42].
The osmotic pressures of PA-Na solutions with different con-
centrations are shown in Fig. 4. The osmotic pressure of the PA-Na
solution increases linearly from 15.56 bar at 0.15 M to 76.38 bar at
0.75 M because a larger number of free ions are ionized in the PA-Na
solution with a higher concentration. Benchmarking in Table S1 also
shows that, the osmotic pressure of the proposed novel PA-Na draw
solution is considerably higher [43–45] compared to those of most
other polyelectrolyte draw solutions with a similar concentration, in-
dicating its great potential for the application in FO.
The FO performance of the PA-Na draw solutions with different
Fig. 4. The osmotic pressure and relative viscosities of PA-Na solutions with
different concentrations (0.15–0.75 M, pH = 7).
90
Desalination 448 (2018) 87–92
Fig. 5. FO performance with PA-Na draw solutions in (a) PRO mode, and (b) FO
mode (pH = 7) (feed solution: DI water).
concentrations in both PRO and FO modes is presented in Fig. 5. The
water fluxes in both modes increase with an increase in draw solution
concentration, attributed to increased osmotic pressure. In addition, the
water flux in the PRO mode is about three times higher than that in the
FO mode with the same draw solution concentration because of the
reduced ICP effect. The PA-Na draw solution with a concentration of
0.75 M obtains the highest water fluxes of 11.67 and 24.55 LMH in the
FO and PRO modes, respectively. The low reverse salt flux also ranges
from 0.18 gMH to 0.39 gMH in the FO mode and 0.43 gMH to 0.82 gMH
in the PRO mode. Fig. 5 also shows that the Js/Jw ratio slightly declines
with an increase in the draw solution concentration from 0.15 M to
0.45 M and then slightly increases with a further increase in con-
centration to 0.75 M in both modes. Regardless, all Js/Jw ratios remain
below 0.04 g/L, attributed to the high water flux and low salt flux.
These results suggest the great potential of PA-Na as a draw solute for
FO.
Owing to the relatively large molecular size of the PA-Na draw so-
lutes used in this study, the FO performance of the PA-Na draw solution
was further evaluated using self-made HPAN-TFC membranes. As
shown in Table 1, both the water flux and reverse draw solute flux of
HPAN-TFC membrane are higher than that of HTI-TFC membrane, in-
dicating that HPAN-TFC membrane is more permeable to both water
and NaCl molecules. It can be seen from Table 3 that with the PA-NA
draw solution (0.45 M), the HPAN-TFC membrane can produce a much
higher water flux than the HTI-TFC membrane while producing only a
slightly higher reverse salt flux, resulting in a much lower Js/Jw ratio.
This result indicates that the performance of PA-Na draw solution with
a relatively large molecular size can be optimized using a more
permeable FO membrane.
J. Huang et al. Desalination 448 (2018) 87–92

Table 3 Table 4
FO performance of different membranes. Relative viscosity of PA-Na and NaCl solutions with different ion molarity.
Membrane Water flux (LMH) Reverse salt flux (gMH) Js/Jw (g/L) Ion molarity (M) PA-Na NaCl

HTI-TFC 19.02 ± 1.63 0.51 ± 0.03 0.0273 ± 0.0004 2.10 5.60 ± 0.13 1.17 ± 0.01
HPAN-TFC 30.35 ± 1.12 0.61 ± 0.05 0.0201 ± 0.0007 2.88 13.22 ± 0.27 1.39 ± 0.01

Note: DI water and 0.45 M PA-Na solution were used as the feed solution and
draw solution respectively; PRO mode. Fig. 6(b) shows the FO performance of the PA-Na and NaCl draw
solutions with the same ion molarity. To produce the same ion molarity
of 0.45 and 0.6 M PA-Na solution, 1.05 and 1.44 M NaCl solutions are
required. As shown in Fig. 6(b), the water flux for PA-Na draw solution
is lower than that for NaCl solution with the same ion molarity, which is
mainly attributed to their different viscosity. As presented in Table 4,
the viscosity of PA-Na draw solution is around 5–10 times higher than
that of NaCl solution. The significantly higher viscosity of PA-Na so-
lution could lead to the much more severe concentration polarization
and the considerable reduction in the effective osmotic driven force,
and therefore the resultant lower flux of PA-Na draw solution. How-
ever, the salt leakage of the PA-Na draw solution is significantly lower
than that of the NaCl solution with the same ion molarity because of the
higher molecular weight of the former.

3.4. Application of PA-Na for brackish water desalination

In this study, the 0.45 M PA-Na solution was further explored as the
draw solution for the desalination application with synthetic brackish
water (0.15 M NaCl) as the feed solution. Fig. 7 shows the variation in
the water flux in a test running for 30 min, with DI water and 0.15 M
NaCl solution as the feed solutions. With DI water as the feed solution,
the water flux achieved with the 0.45 M draw solution is about
5.22 LMH, which is much higher than that achieved with the 0.5 M
NaCl draw solution (2.75 LMH, as shown in Table 1). In addition, when
the feed solution is replaced with the synthetic brackish water, the
water flux decreases to about 2.87 LMH because of the reduced differ-
ence in transmembrane osmotic pressure. Despite the reduction, this
water flux is still considered acceptable and suggests the feasibility of
the PA-Na solution for desalination.
Compared with NaCl draw solution, PA-Na draw solution holds a
greater potential for desalination in terms of the much lower draw so-
lute leakage and the competitive water flux in FO process as shown in
Fig. 6. In addition, since a 0.2–1 wt% PA-Na solution can be used as a
food additive [33–35], the dilute draw solution after desalination

Fig. 6. FO performance of PA-Na and NaCl draw solutions with the same (a)
solute molarity and (b) ion molarity.

3.3. Comparison of PA-Na and NaCl draw solutions

The FO performances of PA-Na and NaCl are compared with the

same solute molarity and the same ion molarity, respectively. Fig. 6 (a)
presents Jw and Js generated with the NaCl and PA-Na draw solutions
of the same solute molarity (0.45 or 0.6 M). The PA-Na draw solution
has a much higher Jw and a lower Js than the NaCl draw solution,
which could be attributed to a large number of free ions dissociated in
the PA-Na solution and the larger molecular weight of PA, respectively.
According to the determined dissociation degree of PA-Na in Table S2,
0.45 and 0.6 M PA can produce 2.10 M (=0.45 ∗ 13 ∗ 0.36) and 2.88 M
(=0.6 ∗ 13 ∗ 0.37) free ions, which are much higher than those gener-
ated by the NaCl solution with the same molarity (0.9 and 1.2 M free
ions generated). A larger number of free ions indicate higher osmotic
pressure and consequently, a higher Jw. Fig. 7. FO water flux with 0.45 M PA-Na draw solution for the brackish water
desalination (HTI-TFC membrane, FO mode).

91
J. Huang et al.
process can be used in the food industry after being diluted to a re-
quired range.
4. Conclusions
In this study, PA-Na as a draw solute for FO is evaluated. The effects
of solution pH and concentration on the osmotic pressure, the relative
viscosity, and the resulting FO performance are systematically studied.
With increases in solution pH and concentration, both the osmotic
pressure and relative viscosity increase with more free ions generated in
the draw solution, contributing to a higher water flux but more severe
salt leakage in FO. With DI water as the feed solution, a high water flux
of 24.55 LMH and a relatively low salt flux of 0.39 gMH can be achieved
using a 0.75 M PA-Na draw solution (pH of 7) in the PRO mode.
Negligible Js/Jw ratios (≤0.04 g/L) can be achieved in both FO and
PRO modes. Meanwhile, the FO performance of the PA-Na draw solu-
tions can be improved using a self-made HPAN-TFC FO membrane.
Owing to the much lower draw solute leakage and the competitive
water flux in FO process, PA-Na draw solution is further explored for
brackish water desalination with a relatively high water flux, indicating
its great potential in this aspect. The diluted PA-Na draw solution after
FO may be used directly in food production by further dilution. In
general, the non-toxicity and satisfactory FO performance of this food
additive demonstrate its great potential as a draw solute for applica-
tions in FO.
Acknowledgement
We would like to acknowledge the financial supports from National
Natural Science Foundation of China (no. 21306058), and the Free
Exploring Fundamental Research Project from Shenzhen Research
Council, China (no. JCYJ20160408173516757).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.desal.2018.10.004.
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