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Ultrafiltration of Banana (Musa acuminata) Juice Using Hollow Fibers for


Enhanced Shelf Life

Article  in  Food and Bioprocess Technology · September 2014


DOI: 10.1007/s11947-014-1309-7

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Food Bioprocess Technol (2014) 7:2711–2722
DOI 10.1007/s11947-014-1309-7

ORIGINAL PAPER

Ultrafiltration of Banana (Musa acuminata) Juice Using Hollow


Fibers for Enhanced Shelf Life
Sorel Tchewonpi Sagu & Sankha Karmakar &
Emmanuel Jong Nso & Cesar Kapseu & Sirshendu De

Received: 11 September 2013 / Accepted: 24 March 2014 / Published online: 22 April 2014
# Springer Science+Business Media New York 2014

Abstract Banana juice was clarified by cross flow ultra- Introduction


filtration using a hollow fiber module under total recycle
mode. Three surface-modified polysulfone-based mem- Natural fruit juice beverages are becoming a regular drink for
brane cartridges with molecular weight cut-offs 10, 27, people around the world. In addition to being rich in nutrients
and 44 kDa were used to identify the most suitable with a wide range of vitamins, minerals, protein, and varied
membrane. The effects of operating conditions—namely, source of protective antioxidants, fruit juices also have the
transmembrane pressure drop and cross flow rate on the ability to impart equivalent energy. Banana fruits (Musa
permeate flux and permeate quality, have been investi- acuminata) are particularly relevant due to their aroma and
gated. The quality of the clarified juice was evaluated in flavor and are classed as one of the most popular fruits in the
terms of viscosity, clarity, color, alcohol insoluble world market (Sulaiman et al. 2011). Banana is a source of
solids, total soluble sugar, pH, protein, and polyphenol carbohydrate, protein, vitamins A and C, potassium, calcium,
content. The results showed that the membrane of mo- sodium, and magnesium (Fabiano et al. 2006). As a pulpy
lecular weight cut-off 27 kDa was suitable. The perme- fruit, banana is also suitable for juice production, but the main
ate flux depended strongly on the transmembrane pres- problem is the high concentration of pectic substances that
sure drop, but its variation on cross flow rate was make the juice cloudy and unstable. Sims and Bates (1994)
insignificant. The clarified juice had high clarity and had processed banana juice by ultrafiltration and pasteuriza-
no pectineous materials (in terms of alcohol insoluble tion to improve its nutritional quality, but in their study, they
solids). It contained significant amount of polyphenol had used additives like potassium sorbate and ascorbic acid.
and protein. The storage study indicated that the juice Sims et al. (1994) has used ultrafiltration and pasteurization
could be successfully stored for 1 month without any for comparing the characteristics of different maturity grade
additive and preservative, keeping its natural nutritional bananas. The comparison of 10- and 30-kDa membrane was
qualities, taste, and flavor intact. done to observe the effect on removal of polyphenol oxidase
and the browning of the juice. But, no throughput was report-
ed. Also, the flavor of the juice was changed significantly due
Keywords Banana juice . Clarification . Ultrafiltration . to pasteurization. In addition to nutritional characteristics,
Hollow fiber membrane transparency and homogeneity are also two essential parame-
ters for desired quality of the final product (Vaillant et al.
2001). Thus, it is necessary to have desired physical charac-
teristics without compromising the nutritional qualities.
S. T. Sagu : E. J. Nso : C. Kapseu
Membrane techniques, being physical processes, appear to
Department of Process Engineering, National School of
Agro-Industrial Sciences (ENSAI), University of Ngaoundere, be effective to accomplish the removal of suspended solids,
P.O. Box 455, Adamawa, Cameroon undesired pectin, and high molecular weight protein from the
juice.
S. Karmakar : S. De (*)
Microfiltration and ultrafiltration offer a quite competitive
Department of Chemical Engineering, Indian Institute of
Technology, Kharagpur, Kharagpur 721302, India and attractive alternative compared to thermal processes that
e-mail: sde@che.iitkgp.ernet.in cause an irreversible change in the flavor profile, color
2712 Food Bioprocess Technol (2014) 7:2711–2722

degradation, and appearance of cooked product (Cassano et al. reversible and irreversible fouling both can occur simulta-
2006). Microfiltration was used as a pretreatment for clarifi- neously. In extracts of fruit juice, fouling is usually caused
cation of pineapple juice (Carvalho and Silva 2010) and cactus by molecular aggregates such as starch, pectin, cellulose,
pear juice (Mondal et al. 2013). The use of ultrafiltration as tannins, and proteins, which are well-known cake-forming
membrane processes for the clarification of fruit juices has agents. Therefore, cake filtration is a dominant mechanism
been the subject of numerous research, such as guava juice of membrane fouling over pore blocking in case of extract of
(Chan and Chaing 1992), passion juice (Jiraratananon and fruit juice (Bhattacharya et al. 2001; Vladisavljević et al.
Chanachai 1996), apple juice (Constenla and Lozano 1997; 2003; Cassano et al. 2006; Emani et al. 2013).
Bruijn et al. 2003; Vladisavljević et al. 2003; Yazdanshenas In the pulpy fruit juices such as banana, this fouling would
et al. 2010), peach, blood orange juice (Cassano et al. 2007a), be significant, primarily due to the insoluble solids consisting
kiwifruit juice (Cassano et al. 2007b), watermelon (Rai et al. of pectic substances and starch. To reduce the membrane
2010a, b), pomegranate juice (Cassano et al. 2011), stevia fouling during the ultrafiltration of pulpy fruit juices, juice is
extract (Chhaya et al. 2012), pear, and mandarin juice usually pretreated with enzymes (Vaillant et al. 1999). Also, a
(Echavarría et al. 2012). Palmu et al. (1999) had used 10- primary clarification stage involving centrifugation or
kDa plate and frame ultrafiltration membrane to remove poly- microfiltration allows an elimination of large part of the par-
phenol oxidase from the banana juice to prevent browning. ticles in the juice and thus greatly improves the permeate flux
But, in this method, they did not remove pectin or other during ultrafiltration (Chhaya and De 2013).
fibrous substances through any primary clarification. Hence, The aim of this work was to achieve clarification of banana
the fouling was significant, and also, the shelf life of the juice by ultrafiltration using polymeric hollow fiber mem-
extracted juice was less. It follows from this literature back- branes for the first time. Enzymatically treated banana juice
ground that ultrafiltration of banana juice leading to high shelf was initially treated by microfiltration as a primary clarifica-
life without any preservative is scant in literature. This is due tion. Membranes of molecular weight cut-offs (MWCOs) 10,
to high content of pectic substances which would result in 27, and 44 kDa were used to select the most suitable mem-
drastic fouling of membrane and reduction in the permeate brane. The effects of cross flow rate and transmembrane
flux. pressure drop on permeate flux were investigated, and some
It is well known that the reduction of permeate flux with parameters of permeate, like clarity, color, viscosity, alcohol
time is the major problem of membrane filtration during insoluble solid (AIS), total soluble sugar (TSS), total dis-
clarification of fruit juice. Decline of permeate flux is due to solved solid (TDS), total polyphenol, and protein, were ex-
membrane fouling (Vladisavljević et al. 2003; Yazdanshenas amined. Finally, the potential of the present study was ex-
et al. 2010; Hamachi et al. 2003; Rai et al. 2006a, b). Fouling plored undertaking a storage study and analyzing the quality
is of two types, namely, reversible and irreversible. In case of and taste of the filtered juice.
reversible fouling, the fouling resistance can completely be
removed after adopting an appropriate cleaning protocol
(Blatt et al. 1970). Reversible fouling is associated with con- Materials and Methods
centration polarization, i.e., accumulation of solute particles
over the membrane surface. Concentration polarization can Enzyme Source and Other Chemicals
lead to several phenomena: (1) increase in solution osmotic
pressure at membrane–solution interface, reducing the effec- Pectinase (EC3.2.1.15) from Aspergillus niger with activity
tive driving force; (2) being a strong increasing function of 3.5–7 units/mg was purchased from M/s, Sisco Research
concentration, viscosity at membrane–solution interface in- Laboratory, Mumbai, India, and used for enzymatic treatment
creases exponentially, thereby offering an extra resistance of banana pulp. Folin–Ciocalteu reagent, anhydrous sodium
against the solvent flux; and (3) deposition of a cake-type carbonate, and copper (II) sulfate pentahydrate were pur-
layer made of larger-sized solute particles over the membrane chased from M/s, Merck Specialities Pvt. Ltd., Mumbai,
surface. All these phenomena lead to a common outcome, i.e., India, and potassium sodium tartarate was obtained from
decline in permeate flux. Irreversible fouling occurs by ad- M/s, Loba Chemie, Mumbai, India. Bovine serum albumin
sorption of solute particles on the pore mouth or inside the was used for calibration for protein estimation, and it was
pores, blocking the pores partially or completely. This leads to procured from M/s, Sisco Research Laboratories Pvt. Ltd,
reduction in membrane permeability and hence the permeate Mumbai, India. Gallic acid standard, used for calibrating
flux. However, even after adopting suitable cleaning mea- polyphenol content was obtained from M/s, Loba Chemie,
sures, a fraction of membrane permeability is not recovered, Mumbai, India. Ethyl alcohol for measurement of alcohol
and there is a permanent loss of permeability (Bungay et al. insoluble solid (AIS) was procured from M/s, Jiangsu Huaxi
1986; Rautenbach and Albrecht 1986; Ho and Sirkar 1992; International Trade Co. Ltd, China. The commercial grade
Cheryan 1998; Porter 2005). In an actual filtration process, filter papers (diameter 110 mm) were procured from M/s,
Food Bioprocess Technol (2014) 7:2711–2722 2713

Whatman, GE Healthcare Ltd., UK. All the glassware used permeability was 5.6×10−11, 5.5×10−10, and 6×10−10 m/
was obtained from M/s, Borosil Glass Works Ltd., Mumbai, Pa.s, respectively, for 10-, 27-, and 44-kDa membranes. The
India. All the chemicals listed above were of analytical grade. suitable MWCO membrane was selected based on the pro-
ductivity and the physico-chemical characteristics of the
Preparation and Primary Clarification of Banana Juice ultrafiltered permeate (clarified juice).

Fresh, mature, and ripe bananas with green skin, commonly Ultrafiltration Experimental Setup
referred to as Dwarf Cavendish Banana variety (Musa
acuminata), were purchased from a local market at A laboratory-scale ultrafiltration unit, with tangential flow and
Kharagpur in West Bengal, India. The extraction process of total recycling of permeate, was used for the clarification of
banana juice was performed according to method described by banana juice (Fig. 1). It was mainly consisted of a feed tank
Sagu et al. (2014). Fresh and ripe bananas were selected, with a capacity of 500 ml, a feed pump, the membrane
washed, peeled, and cut in small pieces. A ratio of 1:2 (ba- module, one pressure valve and one flow control valve, two
nana/water; w/v) was used in the mixing process at 1,000 rpm pressure gauges (at the inlet and outlet of the membrane
for 10 min using a Remi Motor agitator, type RQ 122 supplied module), and one rotameter. Pressure valve on the retentate
by M/s, Elektrotechnik Ltd, Kolkata, India. The mixture was line and flow control valve on the bypass line were used to
put in water bath at 33±2 °C, and then, 0.03 % v/w of adjust the pressure and cross flow rate during the different
pectinase was added, mixed, and then kept for 108 min. ultrafiltration operations. The transmembrane pressure drop
During the incubation period, the mixture was stirred regular- was the average of readings of two pressure gauges across the
ly to allow complete homogenization of the system. At the end membrane module.
of the enzymatic treatment, pectinase was inactivated by
heating at 95 °C for 5 min. The mixture was cooled and Procedure
filtered by a finely meshed cloth to remove pulp. The filtrate
was collected and then directly used for primary clarification After choosing the adequate MWCO membrane, 500 ml of
using cross flow microfiltration. The procedure and the opti- microfiltered banana juice was used for each ultrafiltration
mal conditions were studied using a series of experiment by experiments under the total recycle mode with complete
varying transmembrane pressure drop and cross flow rate. The recycling of the retentate and the permeate stream in the feed
hollow fiber had an effective area of 0.0124 m2. The most tank to maintain the feed concentration uniform. In order to
suitable operating conditions were selected based on the re- investigate the effect of operating conditions on the permeate
lated study and were transmembrane pressure drop 76 kPa and flux and on the characteristics of clarified banana juice, four
cross flow rate 20 l/h. The permeability of membrane was 5× transmembrane pressure drops (35, 52, 69, and 104 kPa) and
10−10 m/Pa.s, and the steady-state flux was 43 l/m2.h. three cross flow rates (10, 15, and 20 l/h) were applied. A total
Microfiltered banana juice was stored at −10 °C and then of 12 experiments were performed until reaching the steady
thawed at room temperature just before use for ultrafiltration state (45 min). Temperature was kept constant at room
experiments. Also, a small sample of permeate (microfiltered
juice) was collected for analysis of TSS, pH, viscosity, clarity,
TDS, AIS, conductivity, the concentration of polyphenol, and
protein.

Clarification by Ultrafiltration

Membranes

To identify the most suitable membrane for the clarification of


microfiltered banana juice, three polymeric ultrafiltration hol-
low fiber cartridges were prepared taking polysulfone as the
base polymer with surface modification. The molecular
weight cut-offs 10, 27, and 44 kDa were used to determine
the suitable membrane. The complete procedure for preparing Fig. 1 Schematic diagram of tangential ultrafiltration unit with recycle
mode. 1 Feed thank; 2 section pipe; 3 feed pump; 4 pressure valve; 5 by-
the hollow fiber module used, its characterization, and perfor- pass pipe; 6 and 6’ pressure gauge (at the inlet and outlet of the membrane
mance were described by Thakur and De (2012). The effective module); 7 membrane module; 8 flow control valve; 9 rotameter; 10 flow
area of the three membranes was 0.026 m 2, and their pipe; 11 permeate; 12 heat exchanger
2714 Food Bioprocess Technol (2014) 7:2711–2722

temperature during all the experiments. A back pressure valve Viscosity, Conductivity, and pH
in the retentate line and a by-pass valve were used to adjust
and maintain the transmembrane pressure drop and cross flow The viscosity of banana juice was determined using an
rate independently. A small quantity of permeate was collect- Ostwald capillary viscometer (M/s, Pisco, Kolkata, India),
ed for analysis of physical (pH, viscosity, color, clarity, TDS, and viscosity was measured at room temperature (30±1 °C).
AIS, conductivity) and nutritional (TSS, concentration of The unit of measurement used for viscosity was millipascal–
polyphenol, and protein) characteristics of clarified banana second. Conductivity and pH values of juice were measured
juice. To recover the initial permeability of membrane, the using a multi parameter pocket tester (M/s, EUTECH
module was cleaned after each experiment by circulating the Instruments Ltd, Singapore). The unit for conductivity is
tap water in the circuit followed by acid solution (HCl, 0.1 N) micro-Siemens per centimeter.
for 45 min. After this, an alkaline wash (NaOH, 0.2 N) was
carried out for another 45 min. At the end of the washing Taste
procedure, tap water and then distilled water were re-
circulated through the module for 35 min. The permeability The taste analysis was done by a series of expert in a nine-
of membrane was measured thereafter using distilled water. point hedonic scale, where the rating varies from 1 (dislike
extremely) to 9 (like extremely) (Ranganna 2005). Then,
rankings were given accordingly. The fiducial limits for
Hedonic rating were calculated and checked whether the
Analysis
hedonic mean score fall above or below the fiducial limit.
The taste analysis was undertaken for the sample that was
Color and Clarity
stored in refrigerator at 4 °C for 4 weeks. The taste analysis
was performed on the basis of appearance, texture, aroma,
Color of the sample was measured by absorbance (A) at a
flavor, color, overall quality, and purchase intention.
wavelength of 420 nm using a spectrophotometer (M/s, Perkin
Elmer, Shelton, CT, USA) (Rai et al. 2006a, b). Clarity was
measured by transmittance (%T) at 660 nm using the same
Storage Study
spectrophotometer (Rai et al. 2006a, b).
The shelf life of the clarified juice is very important to make
Particle Size Analysis the clarification process successful. The storage study was
conducted for 4 weeks. The different parameters like TSS,
Particle size of the microfiltered banana juice and clarified total solids (TS), TDS, clarity, color, total protein, total poly-
banana juice from 44-kDa MWCO membrane was measured phenol, and total pectin content (in terms of %AIS) was
by Zetasizer (model: Zetasizer nano ZS90) supplied by M/s, determined each week to analyze the quality of the juice over
Malvern Instruments, Worcestershire, UK. time.
The experiments were conducted in a cross flow hollow
fiber ultrafiltration module in 27-kDa membrane at the most
Alcohol Insoluble Solids
suitable transmembrane pressure and cross flow velocity. The
whole setup was enclosed in a laminar hood chamber to avoid
AIS is the measure of pectineous substances in banana, and it
any bacterial contamination during collection. All the pipes,
is measured by the available procedure (Ranganna 2005).
pump, and valves were washed with 30 % H2O2 and kept at
80 °C for 15 min to remove any bacteria present. The samples
Total Polyphenol, Protein, and Total Soluble Sugar were collected in borosilicate glass bottles. The glass bottles
were washed with ethyl alcohol and kept in hot air oven for
Total polyphenol was measured using a modified Folin and 15 min at 60 °C. The glass bottles were filled to the brim
Ciocalteu method described by Vasco et al. (2008), using a during the collection without head space. After the collection,
spectrophotometer (M/s, Perkin Elmer, Shelton, CT, USA). the bottles were wax sealed and kept at a refrigerated temper-
The results were expressed as milligrams of Gallic acid equiv- ature of 4 °C.
alent (GAE) per 100 ml. Protein concentration was deter-
mined spectrophotometrically by the same spectrophotometer, Statistical Analysis
according to the dye binding method of Lowry et al. (1951)
with bovine serum albumin as standard. The total soluble Each experiment was conducted in triplicate. For each exper-
sugar content (in °Brix) was determined using an ABBE type iment, three samples were taken. The standard deviation of
refractometer (M/s, Excel International, Kolkata, India). each property parameter is reported in the tables and figures.
Food Bioprocess Technol (2014) 7:2711–2722 2715

Steady state flux


In order to check the significance of parameter values between
operating conditions or the properties of the samples in the

6.1±0.3
(l/m2.h)

54±3.0

44±2.0
storage study, a normal distribution function was used (Miller
and Miller 2007). It had been checked whether the values fall



within μ±σ (where μ is the mean of the sample and σ is the

(mg GAE/100 ml
standard deviation). If majority of the cases fall within±σ, it
was concluded that the difference between samples was

Polyphenol

4.31±0.15
4.07±0.1

7.51±0.3
3.63±0.1
insignificant.

46

43

52
Results and Discussions

Protein (mg/l)

146.6±10

761.4±20
246.4±15

273.8±18
Selection of Membrane of Suitable Molecular Weight Cut-off

81

68

64
Three different membranes with molecular weight cut-offs 10,

Clarity (%)
27, and 44 kDa were used to identify the most appropriate one

98.2±0.6

90.8±0.3
97.3±0.4

95.6±0.5
to carry out the ultrafiltration of microfiltered banana juice.
For this purpose, the same operating conditions (transmem-


brane pressure drop of 69 kPa and cross flow rate of 1 l/h)

0.071±0.002

0.145±0.001
0.089±0.001

0.097±0.003
were used. The physical characteristics (viscosity, clarity, AIS,
TSS), nutritional values of permeate (polyphenol and protein),
Color
and the permeate flux values were used as criterion for
(A)

51

39

33
selection.

0.25±0.01
Table 1 shows the physical and nutritional characteristics of
clarified banana juice as well as the steady-state permeate flux
AIS

100

100

100
(%)

0.0

0.0

0.0
obtained after ultrafiltration for each different MWCO mem-
brane. From this table, it is observed that for each of the three

872±30
789±40

803±35

626±38
MWCO membranes (10, 27, and 44 kDa), the amount of AIS
(mg/l)
TDS

28.2
9.5

8.0
content in permeate is zero, corresponding to 100 % retention.
This observation clearly shows that all the solid particles
Conductivity

suspended in the banana juice mainly consisting of pectin 1215±40


1106±60
(μS/cm)

986±55

900±50

and starch were completely rejected. Generally, the molecular


weight of pectin varies from 50 kDa to over 750 kDa

(Yamaguchi et al. 1995), and it is clear that all three mem-


Table 1 Experimental responses of ultrafiltration for different MWCO

TSS (°Brix)

branes completely reject pectineous components in the juice.


5.9±0.2
4.4±0.1

4.1±0.3

3.3±0.2

It is observed that the values of viscosity and clarity of


25.4

31.0

44.1

permeate are almost same for each membrane. It is known


that clarity, color, and viscosity are directly affected by the
Viscosity (mPa.s)

presence of macromolecules present in banana juice. Since


AIS are completely retained by the membranes, values of
1.14±0.02

1.24±0.04
1.15±0.08

1.14±0.05

viscosity and clarity of the clarified juice are similar. The color
reduction by 10-kDa membrane is maximum, i.e., 51 %
followed by 27 and 44 kDa. These results are in perfect

agreement with Sims et al. (1994) who got a color of 0.290


R0 is observed retention in percent
4.42±0.08

4.45±0.06
4.4±0.06

4.3±0.05

A for 10-kDa and 0.367 A for 30-kDa ultrafiltration mem-


brane. The maximum value of polyphenol (4.31 mg GAE/
pH

100 ml) was obtained with 27-kDa membrane (observed


retention 43 %); the maximum values of protein (273.8 mg/
Microfiltered banana

l, with retention 64 %) and TSS (4.4 °Brix, with retention


25.4 %) were obtained with the 44- and 10-kDa membrane,
respectively. Similarly, it is clearly observed from the table
R0 a (%)

R0 a (%)

R0 a (%)
MWCO

juice

that at the steady state, 27-kDa membrane resulted in the


kDa

highest permeate flux with more than 50 l/m2.h. The permeate


10

27

44

a
2716 Food Bioprocess Technol (2014) 7:2711–2722

flux values were 43 and 8.1 l/m2.h, for the membranes of the concentration of protein in permeate for 27- and 44-kDa
MWCO 44 and 10 kDa, respectively. membranes are almost same.
During transport through the membrane, the pectins, pro- Variation of TSS with MWCO of membrane shows an
tein, and hemicelluloses form a cake type of layer over the interesting trend. Pore blocking is minimal for 10-kDa com-
membrane surface which acts as a dynamic membrane. The pared to 27- and 44-kDa membranes. With sugars having
particle size distribution of microfiltered and clarified banana smaller molecular weight (180 to 343 Da) (Chow and
juice is presented in Fig. 2. It is observed from this figure that Landhausser 2004) compared to polyphenol (500 to
in both the cases, size distribution shows double peak. For 3,000 Da) (Todisco et al. 2002), it may be hypothesized that
microfiltered juice, the maximum size density of the particles they are not rejected by cake layer upfront like polyphenol.
is in the range of 0.55 to 1 nm and from 8 to 20 nm. In the case But, since more membrane pores are blocked in the order of
of clarified juice, the maximum intensity is from 0.55 to 3 nm 10-, 27-, and 44-kDa membranes, permeation of sugar is also
and from 8 to 11 nm. The average pore size of these mem- hindered in that order. It is observed that TSS concentration in
branes is calculated using the empirical correlation (Singh permeate decreases from 4.3, 4.0, and 3.5 °Brix for these
et al. 1998), ravg =16.73×10−10(MWCO)0.557, where, ravg is membranes.
average pore radius in centimeters and MWCO is the molec- The interplay of cake layer and pore blocking is evident
ular weight cut-off of the membrane in dalton. Thus, the from steady-state flux values. For 10-kDa membrane, the cake
average pore diameters of 10, 27, and 44 kDa are 5.6, 10, layer is more compact and has higher thickness compared to
and 13 nm, respectively. In 10-kDa membrane, all the higher- 27- and 44-kDa membrane. Thus, it offers maximum resis-
sized particles (8 to 20 nm) are retained by the membrane and tance against the solvent flux, and the flux value is minimal for
form a compact cake layer that rejects the polyphenol to a this (6.l l/m2.h). For 44-kDa membrane, in addition to cake
significant amount. For 44-kDa membrane, particles around layer, pore blocking is higher compared to 27 kDa, and the
13 nm in the microfiltered juice block the membrane pores, flux (44 l/m2.h) is less with respect to 27-kDa membrane that
followed by a cake formation by the higher-sized particles results to the highest permeate flux (54 l/m2.h) of the three
(beyond 13 nm). This phenomenon was observed by Mondal membranes.
and De (2009). Thus, the combined effects of blocked pores Taking into account the different physical, nutritional char-
and the dynamic self-rejecting cake layer result into less acteristics of permeate and different values of permeate flux,
permeation of polyphenol. In fact, polyphenol concentration 27-kDa MWCO hollow fiber membrane was found as the
in the permeate for 44-kDa membrane is the lowest. On the most suitable to perform the ultrafiltration experiments of
other hand, the 27-kDa membrane that has pore size between microfiltered banana juice.
10 and 44 kDa has the highest permeation of polyphenol.
In case of protein, the trend is clear with the molecular cut-
off of the membranes. As the pore size (or MWCO) of the Effect of the Operating Conditions on the Permeate Flux
membrane increases, more protein are permeated. Although,
Transmembrane Pressure Drop and Cross Flow Rate

20
Figure 3a,b,c shows the profiles of permeate flux for 27-kDa
18 membrane, as a function of transmembrane pressure drop and
16
cross flow rate. For each graph, two main comments can be
made: First, there is a sharp decline in permeate flux during
14 Clarified banana juice by 27 kDa membrane
the first 10 min of the operation of ultrafiltration. The second
Intensity (%)

12 observation is the gradual decline of permeate flux thereafter.


For example, in Fig. 3a, it is observed that when the trans-
10
membrane pressure drop was 69 kPa and the cross flow rate
8 was 10 l/h, the initial permeate flux was about 122 l/m2.h. It
Microfiltered banana juice
6 had quickly decreased up to 69 l/m2.h in the first 10 min. After
the tenth minute, the permeate flux continued to decline
4 slowly, from 69 to 56 l/m2.h after 45 min. These two phenom-
2 ena are well known. The first is due to the blocking of the
membrane pores during the first few minutes of operation.
0
1 10 100 The second is due to the deposition of the particles on the
Particle size (nm) membrane surface, thereby forming a cake-type layer that
Fig. 2 Particle size distribution of microfiltered and clarified banana reduces the efficiency of the operation. Macromolecules in
juice banana juice (pectin, starch) block the pores of the membrane
Food Bioprocess Technol (2014) 7:2711–2722 2717

and then deposit on the membrane surface forming cake layer.


The direct effect is the reduction of the effective area of the
membrane and thus leading to flux decline. Jiraratananon and
Chanachai (1996) had reported a permeate flux of 21 l/m2.h at
a transmembrane pressure of 120 kPa and cross flow rate of
48 l/h for a 30-kDa membrane for clarification of passion fruit
juice. Girard and Fukumoto (1999) has obtained a permeate
flux of 50 l/m2.h at 414 kPa and 3.3-m/s cross flow velocity,
for clarification of apple juice with 20-kDa polysulfone mem-
brane. Cassano et al. (2011) observed a similar trend for
pomegranate juice, i.e., at 96-kPa transmembrane pressure
and cross flow rate of 70 l/h, they obtained a flux of 20 l/
m2.h for 69-kDa membrane. Chhaya et al. (2012) recorded a
steady-state flux of 15 l/m2.h in case of stevia for a 30-kDa
membrane at 30-kPa transmembrane pressure and 120-l/h
cross flow rate.
On the other hand, it was also observed that the permeate
flux increased with transmembrane pressure drop
(Fig. 3a,b,c). It is observed from the figures that at the steady
state, the fluxes were proportional to the pressure drop. After
45 min of ultrafiltration (Fig. 3c), the flux was noted as 45, 50,
60, and 80 l/m2.h when applied transmembrane pressures
were 35, 52, 69, and 104 kPa, respectively. This result is in
perfect agreement with Constenla and Lozano (1997), who
got a permeate flux of 55 l/m2.h for clarification of apple juice
by 50-kDa membrane at 73.5-kPa transmembrane pressure
and 1,200-l/h cross flow rate. Bruijn et al. (2003) obtained a
permeate flux of 88 l/m2.h for clarification of apple juice using
carboserp membrane at 150 kPa and 2-m/s cross flow velocity.
Rai et al. (2010a,b) studied the effect of cross flow velocity
and transmembrane pressure in clarification of mosambi
(Citrus sinensis) using cross flow cell with a membrane of
30-kDa MWCO. They obtained a permeate flux of 10–12 l/
m2.h for 276 kPa and 60–120-l/h cross flow rate.
Effect of cross flow rate is also apparent from Fig. 3. Cross
flow rate limits the growth of the cake layer over the mem-
brane surface due to forced convection and increases the
permeate flux. However, in the present study, variation of
cross flow rate is from 10 to 20 l/h. Reynolds number in each
fiber is in the range of 250 to 500 only. Thus, within this range
of Reynolds number, flux enhancement is marginal.

Effect of Operating Conditions of Ultrafiltration


on Physical and Nutritional Characteristics
of Clarified Banana Juice

Table 2 shows the physical and the nutritional characteristics


of the clarified banana juice for various operating conditions
of ultrafiltration by 27-kDa membrane. During the ultrafiltra-
Fig. 3 Effect of pressure on the permeate flux for the different experi-
ments of ultrafiltration of banana juice as function of time: a flow rate tion process, the variation of transmembrane pressure drop
10 l/h; b flow rate 15 l/h, c flow rate 20 l/h and cross flow rate had different effects on the parameters of
permeate juice.
2718

Table 2 Physico-chemical characteristics of clarified banana juice from ultrafiltration (27 kDa)

No. of experiments Operating conditions pH Viscosity TSS (°Brix) Conductivity TDS AIS Color Clarity Protein Polyphenol
(mPa.s) (μS/cm) (mg/l) (%) (A) (%) (mg/l) (mg GAE/100 ml)
TMP (kPa) Cross flow
rate (l/h)

1 35 10 4.91±0.05 1.09±0.005 4.3±0.05 2,100±12 1500±15 0.0 0.082±0.001 98.4±0.05 177.0±12 3.9±0.07
2 15 4.88±0.04 1.15±0.004 3.9±0.04 2,000±14 1560±16 0.0 0.068±0.001 97.7±0.06 200.4±14 3.4±0.08
3 20 4.86±0.03 1.12±0.006 4.2±0.02 2,110±16 1500±12 0.0 0.085±0.001 97.2±0.06 219.8±13 2.4±0.06
R0 a (%) – – 10.2 – 14.1 100 62 – 74 64
4 52 10 4.78±0.06 1.10±0.003 3.9±0.03 2,100±18 1680±18 0.0 0.067±0.002 98.3±0.08 139.4±11 3.8±0.06
5 15 4.76±0.02 1.09±0.004 4.1±0.01 1,867±15 1320±13 0.0 0.070±0.001 98.2±0.06 177.9±10 3.4±0.05
6 20 4.73±0.04 1.09±0.002 3.8±0.04 1,779±13 1260±11 0.0 0.065±0.005 98.1±0.07 128.7±11 4.7±0.07
R0 a (%) – – 14.5 – 19.8 100 67 – 80 55
7 69 10 4.70±0.06 1.14±0.003 4.1±0.02 1,994±16 1400±11 0.0 0.076±0.002 97.5±0.09 283.3±13 4.0±0.09
8 15 4.72±0.03 1.14±0.002 4.0±0.03 2,060±17 1450±16 0.0 0.073±0.001 96.9±0.06 291.2±14 4.0±0.08
9 20 4.60±0.02 1.11±0.004 4.5±0.03 2,060±17 1470±15 0.0 0.077±0.003 97.2±0.08 261.0±14 3.9±0.08
R0 a (%) – – 8.7 – 18.6 100 63 – 63 55
10 104 10 4.72±0.04 1.15±0.001 4.2±0.05 1,896±14 1330±17 0.0 0.088±0.002 96.9±0.08 196.2±15 3.6±0.05
11 15 4.62±0.05 1.13±0.005 4.3±0.01 1,983±13 1400±12 0.0 0.082±0.004 97.4±0.07 262.9±12 3.5±0.06
12 20 4.61±0.04 1.10±0.002 4.3±0.04 2,030±12 1440±14 0.0 0.081±0.002 97.1±0.07 201.8±13 3.4±0.06
R0 a (%) – – 7.2 – 21.5 100 59 – 71 61
Microfiltered banana juice 4.66±0.02 1.19±0.007 4.6±0.06 2,200±20 1,770±20 0.20±0.01 0.205±0.005 92.8±0.10 757.4±15 8.9±0.10
Enzymatically treated banana juice 4.47±0.03 1.49±0.005 5.9±0.05 2,215±50 1,860±30 0.58±0.04 1.174±0.050 52.3±0.50 1308.6±20 15.4±0.50
Feed 4.7±0.05 – 6.7±0.04 2,200±40 – 2.1±0.03 3.6±0.040 0.06±0.002 1827±30 19±0.60

a
Observed retention in percent, averaged over three cross flow rates
Food Bioprocess Technol (2014) 7:2711–2722
Food Bioprocess Technol (2014) 7:2711–2722 2719

worked on the ultrafiltration of depectinized apple juice using


ceramic membranes with MWCO of 30,000, 50,000, and
300,000 Da.
Viscosity of permeate varied from 1.09 (experiments 1, 5,
and 6) to 1.15 mPa.s (experiments 2 and 10). It was noted that
color and clarity of the clarified juice improved a lot during
ultrafiltration of banana juice. In fact, the values of clarity were
52.3 %T for the enzymatically treated banana juice, 92.8 %T
for microfiltered juice and up to 98.4 % in the clarified banana
juice (experiment 1). Color, in term of absorbance, went from
0.205 (enzymatically treated banana juice) to around 0.068 to
0.088 for clarified juice (Table 2). This corresponds to retention
of color in the range of 59 to 67 %. The recovered total soluble
sugar (TSS) was about 90 % for different experiments of
ultrafiltration and varied from 3.9 to 4.5 °Brix when the feed
(microfiltered banana juice) was 4.6 °Brix. Thus, the retention
Fig. 4 The effect of cleaning procedure on the linear permeability of 27-
of sugar is from 7 to 14.5 % only. Also, the values of juice pH
kDa MWCO hollow fiber membrane as function of number of experi-
ment during the ultrafiltration of banana juice were in between 4.61 to 4.91. All these values show that the
operating conditions (transmembrane pressure drop and cross
flow rate) did not really influence the physical characteristics of
Physico-chemical Characteristics of Permeate permeate during the ultrafiltration.
Various properties varied in a narrow range over different
It was observed that the physico-chemicals characteristics of operating conditions. For example, the range of pH was 4.61
permeate were close for different operating conditions of to 4.91; viscosity, 1.09 to 1.15 mPa.s; TSS, 3.8 to 4.5 °Brix;
ultrafiltration. In Table 2, it is noted that a complete rejection conductivity, 1,779 to 2,390 μS/cm; TDS, 1,260 to 1,680 mg/
of AIS occurred for various operating conditions. This means l; color, 0.067 to 0.088; clarity, 97 to 98.3 %; protein: 177 to
that the AIS found in banana juice was composed of sub- 291 mg/l; and total polyphenol from 2.4 to 4.7 mg GAE/
stances with a higher molecular weight than the cut-off of the 100 ml for the clarified juice. It can be noted that there was
membrane used. In fact, determination of the alcohol insoluble significant increase in clarity from microfiltered juice (93 %).
solids (AIS) in the mature fruits or in the fruit juice is related to Viscosity of clarified juice was less than that of microfiltered
starch, hemicelluloses, fiber, and pectin (Ranganna 2005). In one indicating removal of total solids. The average value of
the case of banana juice, AIS determination consists mainly of TSS for all operating conditions was about 4.2 °Brix which
the determination of pectin and starch, and it is very well was close to microfiltered juice, i.e., 4.6 °Brix. There was
known that the molecular weights of pectins are 50,000 Da significant improvement of color (average over all the operat-
and above (Harding et al. 1991; Varanyanond et al. 1999). ing conditions is 0.08) in the clarified juice compared to the
Thus, the total rejection of pectin occurs, and AIS values in the feed (0.21). In the case of protein, the average value of protein
permeate are zero when 27-kDa ultrafiltration is used. Same concentration was about 210 mg/l. Thus, compared to the
results were found by Yazdanshenas et al. (2010) who used a feed, the retention of protein was about 72 % on an average.
polyvinylidene fluoride membrane with a molecular weight Thus, 72 % of the protein in the microfiltered juice had
cut-off of 18 kDa for the ultrafiltration of raw apple juice at average molecular weight beyond 27 kDa. The average poly-
industrial scale and by Vladisavljević et al. (2003) who phenol concentration at 69 kPa is highest, and it was 4.0 mg

Table 3 Results of storage study

Sample pH Viscosity TSS Conductivity TDS AIS Color Clarity Proteins Polyphenol
(mPa.s) (°Brix) (μS/cm) (mg/l) (%) (A) (%) (mg/l) (mg GAE/100 ml)

Feed 4.47±0.3 1.49±0.02 5.9±0.4 1,912±20 1,280±20 0.58±0.02 1.174±0.005 52.3±0.7 1308.6±40 15.4±0.9
Week 0 4.7±0.1 1.08±0.01 3.9±0.2 1,740±12 1,270±15 0±0 0.064±0.001 98.3±0.1 126.2±5.0 4.8±0.1
Week 1 4.7±0.2 1.08±0.03 3.75±0.1 1,750±15 1,250±18 0±0 0.063±0.005 98.2±0.4 130.8±3.0 4.6±0.2
Week 2 4.6±0.1 1.09±0.02 3.6±0.2 1,740±18 1,260±14 0±0 0.067±0.002 98.1±0.3 135.2±4.0 4.4±0.2
Week 3 4.5±0.3 1.09±0.01 3.5±0.2 1,760±20 1,270±20 0±0 0.068±0.001 98±0.2 140.2±6.0 4.1±0.4
Week 4 4.3±0.1 1.08±0.02 3.2±0.1 1,780±14 1,250±10 0±0 0.07±0.003 97.8±0.5 152.8±3.0 3.9±0.1
2720 Food Bioprocess Technol (2014) 7:2711–2722

GAE/100 ml, i.e., the observed retention is about 55 %. 104 kPa and a flow rate of 20 l/h. The various parameters like
Interestingly, average polyphenol concentration in the perme- TSS, TDS, pH, viscosity, total protein content, total polyphe-
ate increased with transmembrane pressure drop due to en- nol, total pectin content (in terms of %AIS), color, clarity, and
hanced convection toward the membrane, and it was maxi- conductivity were determined initially and after each consec-
mum at 69 kPa. Beyond that, the polyphenol concentration utive week. The results are presented in Table 3.
again decreased due to formation of self-rejecting cake-type It can be observed from this table that the quality of juice
layer over the membrane surface. However, the decrease was remains almost same for 4 weeks. From the normal distribu-
really marginal. From the normal distribution of the parame- tion of the parameters, it was observed that the mean value for
ters, it was observed that the mean value for pH, viscosity, pH, viscosity, TSS, conductivity, TDS, color, clarity, protein,
TSS, conductivity, TDS, color, clarity, protein, and polyphe- and polyphenol were 4.6, 1.1, 3.6, 1,754, 1,260, 0.07, 98, 137,
nol were 4.74, 1.12, 4.13, 2,050, 1,443, 0.08, 97.6, 212, and and 4.4, respectively. The standard deviations of the parame-
3.7, respectively. The standard deviations of the parameters ters were 0.2, 0.01, 0.27, 16.7, 10, 0.003, 0.2, 10.2 and 0.4,
were 0.104, 0.024, 0.21, 169, 114, 0.008, 0.6, 53.5, and 0.545, respectively. Hence, 90 % of the values are lying within±σ,
respectively. Hence, 85 % of the values for pH, viscosity, TSS, and all the values lie within ±1.5σ. Since the deviation was
conductivity, color, protein, and polyphenol were lying within marginal from the mean value, the variation of the parameters
± σ and all the values lie within ±1.5σ. For TDS and clarity, was statistically insignificant.
90 % of the values fall within ± σ and all the rest within ±1.5σ.
Since the deviation was not so prominent from the mean
value, it was concluded that the variation of the parameters Conclusion
were statistically insignificant. Hence, the most suitable oper-
ating conditions, i.e., transmembrane pressure drop 104 kPa Pretreated banana juice was clarified by ultrafiltration under
and cross flow rate 20 l/h with maximum permeate flux 80 l/ total recycle mode using hollow fiber module. Based on the
m2.h, were selected based on the productivity of the mem- performance in terms of permeate flux, i.e., system produc-
brane, rather than the variation of the physico-chemical prop- tivity and permeate quality, hollow fiber cartridge of molecu-
erties of the clarified juice. lar weight cut-off 27 kDa was selected as the most suitable
membrane. Transmembrane pressure drop had significant ef-
Taste fect on the permeate flux. At 104-kPa pressure, the permeate
flux can be as high as 82 l/m2.h. The effects of cross flow rate
The fiducial limits for Hedonic rating were calculated as 0.678 on permeate flux were insignificant in the range of 10 to 20 l/
to 1.822 at 1 % and 0.8644 to 1.6356 at 5 % for a control h. The clarified juice contained almost the full amount of TSS
sample. All the mean values for appearance, texture, aroma, of the pretreated juice. AIS values indicated that the concen-
flavor, color, and overall quality on a hedonic scale were tration of pectineous substances in the clarified juice was nil.
below the fiducial limit. Hence, the clarified juice was abso- The clarity was as high as 97 %. The effects of operating
lutely fine after 4 weeks of storage. All the persons taking part conditions on the quality parameters of the clarified juice were
in the rating process confirmed positive purchase intention. marginal. About 50 % of polyphenol and 45 % of protein in
The mean scores of the samples on the basis of texture, aroma, the juice were present in the product. The storage study
flavor, color, and overall quality were 0.37, 0.74, 0.37, 0.37, indicated that the treated juice can be stored for 1 month,
and 0.48, respectively. maintaining the nutritional qualities and taste without adding
any preservatives under refrigerated condition.
Efficacy of Cleaning Procedure
Acknowledgments We acknowledge and thank the Federation of Indian
During the operation of ultrafiltration, the same hollow fiber Chambers of Commerce & Industry (FICCI), the Department of Science &
membrane of 27-kDa MWCO was used for different experi- Technology (DST), and the Ministry of External Affairs (MEA), Govern-
ment of India, for awarding the author Sorel Tchewonpi Sagu, the C V
ments. After every experiment, they were cleaned in situ, and
Raman fellowship for African researcher, to work at the Department of
the permeability of membrane was measured. Figure 4 shows Chemical Engineering, IIT Kharagpur, West Bengal, India.
the variation of permeability as function of different experi-
ments. It is observed that permeability did not change signif-
icantly due to the efficiency of the cleaning protocol. References

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