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Article history:
Received 25 November 2010
Received in revised form 11 January 2011
Accepted 5 April 2011
Available online 12 April 2011
Keywords:
Forward osmosis
Pineapple juice
Anthocyanin
Betalains
Concentration polarization
a b s t r a c t
The possible mechanism of water transport from feed to osmotic agent side during forward osmosis in
situation when feed contains high or low molecular weight compounds and their combination has been
presented. The orientation of membrane was found to inuence the transmembrane ux. When the feed
contains mixture of low and high molecular weight compounds mode I (feed towards the support layer)
was found to result in lower ux values as compared to Mode II (feed towards active layer) due to signicant external concentration polarization. Forward osmosis resulted in the concentration of betalains
content in beetroot juice and anthocyanin content in grape juice from 50.92 mg/L to 2.91 g/L (57.1 fold)
and from 104.85 mg/L to 715.6 mg/L (6.8 fold), respectively. Total soluble solids in case of beetroot, grape
and pineapple juice were found to increase from 2.3 to 52 Brix, from 8.0 to 54.6 Brix from 4.4 to 54
Brix, respectively.
2011 Elsevier Ltd. All rights reserved.
1. Introduction
Fruit juices and natural food colorants are of high nutritive value as they are naturally enriched with minerals, vitamins and
other benecial components required for human health. Removal
of water helps in reducing the water activity, thereby facilitating
the increase in the shelf life of these liquid foods. Hence, it is desirable to concentrate these liquid foods to improve shelf life, stability
and to reduce storage/transportation costs (Babu et al., 2006;
Nayak and Rastogi, 2010a,b). Many researchers have reported forward osmosis for many industrial applications like food processing
(Beaudry and Lampi, 1990; Wong and Winger, 1999) or desalination (Gray et al., 2006).
Membrane processes such as microltration, ultraltration and
reverse osmosis are often being employed for clarication and concentration of fruit juices. The limitations of these membrane processes are attainable maximum concentration (only up to 2530
Brix), concentration polarization and membrane fouling. Conventional method for concentration such as evaporation results in
product deterioration with respect to loss of avors, taste and
nutritive components resulting in low quality product, besides
being energy intensive.
Forward osmosis concentration is a membrane process, which
has potential to concentrate liquid foods/natural colors at ambient
temperature and pressure without signicant product deterioration (Cath et al., 2006; Cath, 2010; McCutcheon and Elimelech,
Corresponding author. Tel.: +91 821 2513 910; fax: +91 821 2517 233.
E-mail address: nkrastogi@cftri.res.in (N.K. Rastogi).
0260-8774/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jfoodeng.2011.04.006
2. Theoretical considerations
In forward osmosis process, the feed and the osmotic agent
solutions are circulated on either side of the semi-permeable
asymmetric hydrophilic membrane. The difference in osmotic
pressures between the feed as well as osmotic agent solutions sets
in the driving force for the ux to occur. There are two possible orientations in which the membrane can be positioned between the
feed and the osmotic agent solutions such as feed towards the support layer and feed towards active layer, which are referred, in the
present work, as modes I and II, respectively.
In case of mode I (Fig. 1a), when the feed is pure water, it is diffused into the support layer and transferred to the osmotic agent
side through the active layer of membrane. No external concentration polarization (ECP) or internal concentration polarization (ICP)
take place on the feed side. An insignicant external polarization
may take place in the boundary layer on osmotic agent side. In this
situation, if the feed (water) consists of solution of low molecular
(a)
OA Side
Feed Side
OA
13, 23
E1 E2
22
21
12
11
feed
Mode I
(b)
OA Side
Feed Side
OA
33
49
32
E3
31
feed
Mode II
Fig. 1. Mechanism of forward osmosis indicating water transport from the solution
of low osmotic pressure to the solution of high osmotic pressure. (a) Mode I: Feed
solution containing low (solid) and mixture of low and high molecular weight
compounds (dotted); (b) Mode II: Feed solution containing low/high molecular
weight compounds. DpE1, DpE2 and DpE3 are the corresponding effective driving
force, respectively. pFeed and pOA are the osmotic pressures of feed and osmotic
agent solution, respectively (Nayak and Rastogi, 2010a).
50
3.2. Extraction
Anthocyanin contentmg=L
A M DF 103
e1
where A480 and A540 refer to the absorption maxima at 540 nm and
480 nm, respectively.
The concentrated extract samples were diluted to original concentration with distilled water before the color measurement and
the values are reported after multiplication with appropriate dilution factor. All the experiments were carried out in triplicates and
average values are reported.
3.5. pH measurement and total soluble solids
pH meter (Eutech 510, Singapore) was used for the measurement of the pH of anthocyanins extract. Total soluble solid of extract was measured using Ermas Handheld refractometer at
25 2 C.
3.6. Membrane experimental setup
Experiments were performed using a at membrane module
having a membrane area of 1.14 102 m2. The module consisted of membrane, which is placed over a polyester mesh (as
a spacer to increase turbulence), supported in between Viton
gasket and two stainless steel frames. Feed solution and osmotic
agent solution were circulated on either side of the membrane in
co-current mode using peristaltic pumps (Model 72-315-230,
Barnant Company, IL, USA). The ratio of feed solution to osmotic
agent solution was maintained at 1:10 for all the experiments.
The transmembrane ux was calculated by measuring the increase in volume of osmotic agent every hour. All the experiments, unless otherwise indicated, were carried out at the
temperature of 25 2 C.
Transmembrane ux was evaluated for water as the feed and sodium chloride as an osmotic agent. The initial transmembrane ux
in case of modes I and II was found to be 19.33 and 9.93 L/m2 h,
respectively. The transmembrane ux was more in case of mode I
as compared to that of mode II. The higher ux in case of mode I
is attributed to the absence of external and internal concentration
polarizations. Whereas, in case of mode II, osmotic agent side internal concentration polarization was found to be signicant due to
setting up of concentration gradient within the support layer.
4.2. Effect of molecular weight of feed solution on transmembrane ux
The effect of molecular weight of feed solution on transmembrane ux was evaluated. The model systems containing different
molecular weight sugars (i.e. 0.15 M dextrose, molecular weight
180 g/mol or 0.15 M sucrose, molecular weight 342.30 g/mol) were
used as feed solutions.
In case of mode I, the transmembrane ux was found to decrease
from 8.94 to 5.38 L/m2 h and from 5.95 to 3.73 L/m2 h for 0.15 M
dextrose and 0.15 M sucrose, respectively (Fig. 2a). The transmembrane ux was found to be higher when 0.15 M solution of dextrose
was taken as a feed solution in comparison to the same concentration of sucrose solution. It is due to the higher penetration power (in
loosely bound support layer) of dextrose (i.e. molecular weight
180 g/mol) in comparison to sucrose (i.e. molecular weight
342.30 g/mol) due to lower molecular weight. The penetration of
low molecular weight compounds (dextrose or sucrose) in the support layer resulted in internal concentration polarization. The extent of which was higher in case of sucrose than that of dextrose.
In case of mode II, the transmembrane ux was found to decrease from 11.03 to 7.20 L/m2 h and from 11.16 to 7.90 L/m2 h
for 0.15 M dextrose and 0.15 M sucrose, respectively (Fig. 2b).
The higher ux in mode II has been reported in case of concentration of fruit juices (Beaudry and Lampi, 1990; Wrolstad et al.,
1993), colorants (Nayak and Rastogi, 2010a,b), sucrose
(Garcia-Castello et al., 2009), and desalination (How et al., 2006;
51
10
M)moles)
Dextrose ((0.15
0.146
M)moles)
Sucrose (0.15
( 0.146
8
6
4
2
(a)
0
0.0
1.0
2.0
3.0
4.0
5.0
6.0
Time (h)
14
Dextrose (0.15
( 0.146
M)moles)
12
M)moles)
Sucrose (0.15
( 0.146
10
8
6
4
(b)
2
0
1.0
3.0
4.0
5.0
6.0
14
60
Cycle 1Cycle 2
12
50
Flux
Brix
10
40
30
20
4
2
0
0.0
Brix
Fig. 2. Variation of ux for dextrose and sucrose for mode I (feed towards support
layer) and mode II (feed towards active layer).
Time (h)
(a)
2.0
4.0
6.0
8.0
10.0
12.0
10
0
Sucrose+dextrose+pectin
0.15
M Dextrose + 0.15 M Sucrose
+ 0.1% Pectin (System III)
6
4
2
(a)
0
0.0
2.0
3.0
4.0
5.0
6.0
12
Cycle 1
Cycle 2
10
50
40
6
4
30
Flux
Brix
20
2
0
0.0
3.0
6.0
Dextrose+pectin
0.15 M Dextrose + 0.1% Pectin (System I)
10
Sucrose+dextrose+pectin
0.15 M Dextrose + 0.15 M Sucrose
+ 0.1% Pectin (System III)
8
6
4
2
(b)
1.0
2.0
3.0
4.0
5.0
6.0
Time (h)
Fig. 3. Variation of ux for combination of sucrose, dextrose and pectin (a) mode I
(feed towards support layer); (b) mode II (feed towards active layer).
Sucrose+pectin
0.15
M Sucrose + 0.1% Pectin (System II)
0.0
9.0
12.0
15.0
18.0
Time (h)
12
10
(b)
Time (h)
14
60
Cycle 3
Brix
Sucrose+pectin
0.15 M Sucrose + 0.1% Pectin (System II)
10
C ycl e 1
Cycle 2
60
C ycl e 4
Cycle 3
50
Flux
Brix
40
30
4
20
2
0
0.0
Brix
10
Time (h)
(c)
3.0
6.0
9.0
12.0
15.0
18.0
21.0
10
0
24.0
Time (h)
Fig. 4. Variation of ux for real food systems (a) beetroot, (b) pineapple, (c) grape
juice.
52
in Fig. 2b. It is due to the enhanced external concentration polarization because of presence of pectin. It may be noted that in mode
II there exists no internal concentration polarization and additional
external polarization is exerted due to presence of pectin molecule,
which is expected to be same in case of system I and II due to same
concentrations. However, in case of system III the ux were still
lower due to combination of 0.15 M dextrose and 0.15 M sucrose
leading to higher effective concentration on feed side thereby
reducing the effective driving force (Fig. 3b).
These results clearly indicate that mode II can be considered as
the best possible orientation with regard to forward osmosis membrane for the concentration of feed containing mixture of low/high
molecular weight compounds (i.e. fruit juices) in food processing.
4.4. Concentration of real food systems
The real food systems (beet, pineapple or grape juice) were concentrated using mode II in cycles of forward osmosis concentration.
Six hours of continuous concentration was referred as a cycle. Since
in case of real food systems, the uxes were reducing very signicantly after 6 h, the membrane was washed with distilled water
after each cycle and next cycle was continued. The variation in
the ux and Brix in each case is presented in Fig. 4. For all the real
systems, the uxes were found to decrease in the each cycle, but
these were found to increase in the beginning of next cycle. The
beetroot juice was concentrated in 2 cycles and the betalains content of the juice was found to increase from 50.92 mg/L to 2.91 g/
L (57.1 fold) and total soluble solids was found to increase from
2.3 to 52 Brix (22.6 fold) (Fig. 4a). The pineapple juice was concentrated in 3 cycles and the total soluble solids was found to increase
from 4.4 to 54 Brix (12 fold, Fig. 4b). The anthocyanin from the
grape juice was concentrated in 4 cycles from 104.85 mg/L to
715.6 mg/L (6.8 fold) and total soluble solids from 4.4 to 54 Brix
(12.3 fold) (Fig. 4c). Maximum anthocyanin concentration of 4.5,
7.5, and 54-fold have been reported in case of red raspberry
Wrolstad et al. (1993), red radish Rodriguez-Sanoa et al. (2001)
and Garcinia indica Choisy (Nayak and Rastogi, 2010a), respectively.
5. Conclusion
Forward osmosis process can be potentially used for the concentration of fruit juices especially in the case when the fruit juice
contains various sugars and heat sensitive compounds such as
betalain or anthocyanin. In case of a model food system consisting
of dextrose, sucrose and pectin, the membrane orientation such
that feed was towards active layer was found to result in higher
transmembrane ux. Forward osmosis resulted in the concentration of betalains content in beetroot juice from 50.92 mg/L to
2.91 g/L (57.1 fold increase) and anthocyanin content in grape juice
from 104.85 mg/L to 715.6 mg/L (6.8 fold). Total soluble solids in
case of beetroot, grape and pineapple juice were found to increase
from 2.3 to 52 Brix (22.6 fold), from 8.0 to 54.6 Brix (6.85 fold)
and from 4.4 to 54 Brix (12.3 fold), respectively.
Acknowledgements
Authors thank Dr. V. Prakash, Director, CFTRI, Mysore for his
encouragement. Thanks are also due to Dr. KSMS Raghavarao,
Head, Department of Food Engineering, CFTRI for his support. The
author Chetan A Nayak expresses his gratitude and sincere thanks
to the Council of Scientic and Industrial Research (CSIR), New Delhi for providing Senior Research Fellowship. The authors also thank
Dr. Edward G. Beaudry, Director of Process Development, Hydration Technology Innovations, USA for providing us forward osmosis
membranes to continue the work further in this direction.
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