chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632

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Chemical Engineering Research and Design

journal homepage: www.elsevier.com/locate/cherd

Microencapsulation of Morinda citrifolia L. extract by

spray-drying

Duduku Krishnaiah ∗ , Rosalam Sarbatly, Rajesh Nithyanandam

Phytochemical Laboratory, Department of Chemical Engineering, School of Engineering and Information Technology, Universiti Malaysia
Sabah, 88999 Kota Kinabalu, Malaysia

a b s t r a c t

Microcapsules containing Morinda citrifolia L. microparticles were produced by a spray-drying technique using various
proportions of ␬-carrageenan and maltodextrin as the binding materials. In this work, the effects of spray-drying
on the encapsulation yield, particle size, moisture content, DPPH scavenging activity, total phenolic content and
total flavonoid content of the bioactive components of M. citrifolia L. were determined for different volume ratios in
the inlet air temperature range of 90–140 ◦ C. The results showed that the percentage of 2,2-diphenyl picrylhydrazyl
(DPPH) scavenging activity of the spray-dried powder was the highest for the 1:2 ratio (volume ratio of M. citrifolia L.
extract to additive solution) at 90 ◦ C, with maltodextrin at a concentration of 33 mg/ml. The results also showed that
the microcapsules had a regular spherical shape. The spray-dried M. citrifolia fruit extract showed high antioxidant
activity (28.36% DPPH activity), thus suggesting that it might be useful as a food additive and/or ingredient under the
above optimum operating conditions.
© 2011 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.

Keywords: Morinda citrifolia; Microencapsulation; Spray-drying; ␬-Carrageenan; Maltodextrin

1. Introduction
Morinda citrifolia L. (noni) has been used in traditional Polyne-
sian medicine for more than 2000 years. This plant belongs to
the family Rubiaceae and is commonly found in the Hawaiian
and Tahitian islands. The bark, stem, root, leaf and fruit have
been traditionally used as folk remedies for many diseases,
including diabetes, hypertension and cancer (Hirazumi et al.,
1994, 1996). In traditional pharmacopoeia, M. citrifolia L. fruit
is claimed to prevent and cure several diseases. It is primarily
used to stimulate the immune system and thus to fight bac-
terial, viral, parasitic and fungal infections. It is also used to
prevent the formation and proliferation of tumours, including
malignant ones (Dixon et al., 1999; Earle, 2001).
Levand and Larson (1979) identified several compounds
including acetyl derivatives of asperuloside, glucose, caproic
acid and caprylic acid in M. citrifolia L. fruits. Wang et al. (1999)
isolated two glycosides, rutin and asperulosidic acid, and a
novel trisaccharide fatty acid ester from M. citrifolia L. fruits.
Carboxylic acids, especially octanoic acid and hexaonoic acid,
have also been identified in the fruits. A total of 51 volatile
compounds have also been found in the ripe fruit (Sang et al.,
2001) including organic acids (Farine et al., 1996). Based on the
literature, it is clear that the fruit has antibiotic and antioxi-
dant properties, but there is a lack of scientific evidence based
on in vivo studies. Because M. citrifolia L. is believed to have
high antioxidant potential, it may substitute as an antioxidant
compound in food items and in preventive medicines. In our
recent work, the antioxidant potentials of various medicinal
plant species were reviewed (Krishnaiah et al., 2011).
Spray-drying is a well-established and widely used tech-
nique for transforming liquid foods or suspensions into a
powder in a one-step process. The microencapsulation tech-
nique of spray-drying is an effective way to protect drug or food
ingredients against deterioration and volatile losses. The pro-
tective mechanism consists of the formation of a membrane
wall that encloses droplets or particles of the encapsulated
material. The choice of a particular method depends on the
type of microparticles desired. The properties of the wall struc-
tures, size and shape are important considerations. However,
in the food and drug industry, spray-drying is still the most
popular method of forming microparticles because it is very

∗
Corresponding author. Tel.: +60 88 320000x3059; fax: +60 88 320348.
E-mail address: krishna@ums.edu.my (D. Krishnaiah).
Received 18 April 2011; Received in revised form 2 August 2011; Accepted 5 September 2011
0263-8762/$ – see front matter © 2011 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.cherd.2011.09.003
 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632
easy to industrialise and allows for continuous production
(Su et al., 2008). Hence, many researchers have used spray-
drying techniques for the production of microparticles of fruit
extracts (Tonon et al., 2010; Saenz et al., 2009; Kha et al.,
2010; Goula and Adamopoulos, 2010). In our previous study,
a preliminary data of spray dried M. citrifolia L. fruit extract
with ␬-carrageenan was reported (Krishnaiah et al., 2009). For
microencapsulation by spray-drying, carrageenan is a good
choice as the wall material due to its pseudoplastic proper-
ties. These properties allow it to act as a plasticiser, promoting
the formation of spherical and smooth-surfaced microcap-
sules and enhancing the adhesion force between the wall and
the core materials (Su et al., 2008). Moreover, it has the desir-
able properties of emulsification, edibility and biodegradation.
Similarly, hydrolysed starches, called maltodextrins, are often
used as wall materials due to their low cost, bland flavour, high
water solubility (up to 75%) and low viscosity when in solu-
tion (Turchiuli et al., 2005). Maltodextrins are mainly used to
reduce stickiness and agglomeration problems during storage,
thereby improving product stability (Bhandari et al., 1993).
The aim of this work was to elucidate the effect of two adju-
vants on the spray-drying of M. citrifolia L. fruit extract and to
find the optimal processing parameters of spray-drying to cre-
ate powdered M. citrifolia L. extract with the highest free radical
scavenging activity, total phenolic content and total flavonoid
content as well as with the optimal particle size and moisture
content.
2. Materials and methods
2.1. Chemicals
Methanol and ethyl acetate (HPLC grade) were obtained from
J.T. Baker (USA). Folin Ciocalteau reagent and tannic acid (TA)
were purchased from Merck, Germany. The chemicals 2,2-
diphenyl picrylhydrazyl (DPPH), aluminium trichloride (AlCl3 )
the weight of microparticles after spray drying
EY% =
total weight of adjuvants and Morinda citrifolia L. powder added initially
and sodium carbonate were obtained from Sigma Chemicals
(St. Louis, USA). A total of 5 kg of M. citrifolia L. fruit before
the ripening stage was obtained from Kota Kinablu, Sabah,
Malaysia. All other chemicals were of reagent grade and were
used without further purification.
2.2. Preparation of plant extracts
M. citrifolia L. fruit was washed with tap water followed by
washing with distilled water. The fruit was peeled, and the
core (pulp and seed) was cut into small species. The skin,
pulp and seed were sun-dried for two days. Then, the sam-
ple was kept at 60 ◦ C in a hot-air oven for one day to remove
all moisture. The dried fruit was then finely powdered using
a mixer. A total of 250 ml of ethyl acetate was added to 25 g of
powdered sample (10 wt%), and extraction was performed in
a water shaker bath at 35 ◦ C for three days. The supernatant
was then separated from the residue by filtration using What-
man no. 1 filter paper. The extracted solution was stored in a
closed container and kept at 4 ◦ C before being analysed. Con-
centrated fruit extract was prepared by taking 200 ml of fruit
extract and subject to rotary evaporator with 60 rpm for 24 h
at 90 ◦ C.
623
2.3. Spray-drying of the M. citrifolia L. fruit extract
␬-Carrageenan (1 wt%) and maltodextrin (5 wt%) were mixed
with M. citrifolia L. fruit extract at different volume ratios (1:1,
1:2, 1:4 and 1:6 for ␬-carrageenan and 1:1, 1:2, 1:3 and 1:4 for
maltodextrin) and then stirred with a mechanical agitator in
a water bath shaker at 100 rpm to form an aqueous solution
(Artur and David, 2001; Turchiuli et al., 2005). The resulting
mixture was then spray-dried using a lab plant spray-dryer
SD-05 (pilot scale) with co-current flow (the spray-dried prod-
uct and the drying air flow were in the same direction). The
drying chamber had a diameter of 215 mm and a height of
500 mm. The main components of the system were the feed
system of the M. citrifolia L. fruit extract consisting of a peri-
staltic pump, a fluid atomiser (inlet orifice diameter of 0.5 mm)
and an air compressor as well as a feed system for drying the
gas consisting of a blower and an air filter. Finally, an inlet
air temperature control system and a product control system
(cyclone) were also employed. The feed flow rate was kept at
315 ml/h. The flow rate of the drying air was fixed at 60 m3 /h,
and the atomising air remained at a pressure of 1.1 bar. After
spray-drying, the powders were collected through a high effi-
ciency cyclone in a glass container, transferred to a glass vial
and stored in desiccators at ambient temperature.
Several spray-drying runs were carried out to investigate
the effects of the inlet air temperature for different volume
ratios of M. citrifolia L. fruit extract to excipient as shown in
Tables 1 and 2. Further analyses were performed to determine
the antioxidant activity, the total phenolic content and the
total flavonoid content of the spray-dried powder.
2.4. Encapsulation yield (EY)
The encapsulation yield was calculated as the ratio of the mass
of the microcapsules obtained at the end of the process to the
mass of the initial substances added including the adjuvant
and M. citrifolia L. powder (Su et al., 2008).
× 100
2.5. DPPH radical scavenging activity
DPPH is a stable free radical that reacts with compounds that
are able to donate a hydrogen atom. Thus, the hydrogen donat-
ing abilities of concentrated M. citrifolia L. fruit extract and
spray-dried M. citrifolia L. fruit extract were determined from
the change in absorbance at 515 nm by the Blois (1958) method
with slight modifications. For free radical scavenging mea-
surements, samples in methanol solution were prepared by
dissolving 10 mg of spray-dried powder in 30 ml of methanol
and centrifuging for 10 min using a Sartorius Sigma 3-18 K
centrifuge. Aliquots of supernatant were added to 3 ml of
0.025 g/l DPPH in methanol. The change in absorbance was
measured after 40 min at room temperature using a 4802 UV-
VIS double-beam spectrophotometer. Methanol was used as
the reference. DPPH (0–100 mg/l) was used to obtain a standard
calibration curve. All measurements were made in triplicate.
The DPPH radical scavenging activity in terms of a per-
centage was calculated according to the following equation:
 
Abs515 sample
DPPH scavenging activity (%) = 1 − × 100
Abs515 DPPH solution
 624
Table 1 – Encapsulation yield, particle size distribution, moisture content, percentage of DPPH scavenging activity, total phenolic content and total flavonoid content of spray-dried
microparticles (␬-carrageenan).

chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632

S. no. Ratio Mcore /Mwall Temperature (◦ C) EY (%)a Mean particle Moisture % of DPPH TPC (mg of Total flavonoid content
diameter (␮m)a contenta scavenging activitya TAE/g of SDP)a (mg of CE/g of SDP)a

1 1:1 90 13.07 ± 0.57G 3.82 ± 0.05B 0.129 ± 0.005B 15.85 ± 0.80EF 21 ± 0.005E 22.5 ± 0.004C
2 1:1 100 16.80 ± 0.80F ND 0.082 ± 0.002EF 11.00 ± 0.85GH 18 ± 0.005F 17.5 ± 0.004D
3 1:1 120 11.86 ± 0.14GH ND 0.067 ± 0.005GH 7.00 ± 0.96I 15 ± 0.009G ND
4 1:1 140 48.13 ± 0.50A ND 0.054 ± 0.006I 4.50 ± 0.94J ND ND
5 1:2 90 31.56 ± 0.50B 2.27 ± 0.04G 0.137 ± 0.006AB 24.91 ± 1.11A 36 ± 0.006A 30.0 ± 0.008A
6 1:2 100 26.04 ± 1.40D 3.96 ± 0.02A 0.095 ± 0.008D 19.57 ± 1.20C 24 ± 0.004D 27.5 ± 0.002B
7 1:2 120 20.73 ± 1.03E 3.69 ± 0.08C 0.075 ± 0.009EFG 14.24 ± 0.98F 12 ± 0.009H ND
8 1:2 140 7.71 ± 1.70J ND 0.055 ± 0.005I 9.64 ± 0.94H ND ND
9 1:4 90 11.20 ± 1.20HI 3.48 ± 0.06D 0.141 ± 0.002A 21.66 ± 1.21B 27 ± 0.004C 27.5 ± 0.004B
10 1:4 100 31.42 ± 1.00B 2.64 ± 0.05F 0.107 ± 0.004C 16.76 ± 1.13DE 24 ± 0.004D 22.5 ± 0.004C
11 1:4 120 5.15 ± 0.85K ND 0.080 ± 0.006EF 11.94 ± 1.15G 21 ± 0.004E ND
12 1:4 140 27.96 ± 1.00C 2.61 ± 0.01F 0.060 ± 0.007HI 6.24 ± 1.09IJ ND ND
13 1:6 90 19.33 ± 1.00E 3.20 ± 0.05E 0.145 ± 0.009A 25.32 ± 0.99A 36 ± 0.009A 30.0 ± 0.007A
14 1:6 100 16.07 ± 1.07F 2.65 ± 0.09F 0.114 ± 0.005C 18.00 ± 0.93CD 30 ± 0.007B 27.5 ± 0.008B
15 1:6 120 9.96 ± 1.08I ND 0.085 ± 0.004E 11.00 ± 0.91GH 24 ± 0.004D ND
16 1:6 140 6.44 ± 0.56JK ND 0.072 ± 0.001FG 5.00 ± 0.85J ND ND

SDP, spray-dried particle; ND, not determined.

Means with same letter in the same column (A–K) are not significantly different (p < 0.05).
a
Reported values are the means ± S.D. (n = 3).
Table 2 – Encapsulation yield, particle size distribution, moisture content, percentage of DPPH scavenging activity, total phenolic content and total flavonoid content of spray-dried

chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632

microparticles (maltodextrin).
S. no. Ratio Mcore /Mwall Temperature (◦ C) EY (%)a Mean particle Moisture % of DPPH TPC (mg of Total flavonoid content
diameter (␮m)a contenta scavenging activitya TAE/g of SDP)a (mg of CE/g of SDP)a

1 1:1 90 20.74 ± 0.26J 3.96 ± 0.05C 0.143 ± 0.006A 18.58 ± 0.86D 33 ± 0.009C 35.0 ± 0.009D
2 1:1 100 32.59 ± 1.09D 2.65 ± 0.02E 0.116 ± 0.009CD 13.30 ± 0.82FG 27 ± 0.006E 30.0 ± 0.009F
3 1:1 120 20.74 ± 0.06J 2.27 ± 0.04F 0.090 ± 0.008FG 9.56 ± 0.50I 21 ± 0.005F ND
4 1:1 140 20.74 ± 0.44J ND 0.071 ± 0.009HI 5.44 ± 0.71K ND ND
5 1:2 90 27.64 ± 0.50G 4.82 ± 0.08A 0.133 ± 0.004AB 28.36 ± 0.80A 54 ± 0.006A 45.0 ± 0.004A
6 1:2 100 25.34 ± 0.34H ND 0.104 ± 0.006DE 22.62 ± 0.97BC 39 ± 0.008B 37.5 ± 0.002C
7 1:2 120 25.34 ± 0.26H ND 0.089 ± 0.005FG 16.24 ± 1.24E 30 ± 0.005D ND
8 1:2 140 39.16 ± 0.66A 2.27 ± 0.09F 0.066 ± 0.007IJ 11.90 ± 0.76GH ND ND
9 1:3 90 37.4 ± 1.00B 3.48 ± 0.07D 0.124 ± 0.005BC 21.42 ± 0.50C 39 ± 0.004B 37.5 ± 0.007C
10 1:3 100 29.09 ± 0.59F ND 0.099 ± 0.003EF 16.36 ± 0.97E 30 ± 0.009D 32.5 ± 0.009E
11 1:3 120 31.16 ± 0.26E ND 0.071 ± 0.009HI 11.64 ± 0.91H 21 ± 0.008F ND
12 1:3 140 14.54 ± 0.94K ND 0.062 ± 0.008IJ 7.16 ± 1.10J ND ND
13 1:4 90 23.53 ± 1.03I 4.27 ± 0.09B 0.116 ± 0.008CD 23.80 ± 1.21B 39 ± 0.004B 40.0 ± 0.009B
14 1:4 100 37.25 ± 0.85B 3.96 ± 0.04C 0.083 ± 0.009GH 18.52 ± 0.80D 33 ± 0.002C 35.0 ± 0.009D
15 1:4 120 35.29 ± 0.71C 3.48 ± 0.04D 0.056 ± 0.006J 13.80 ± 0.60F 27 ± 0.004E ND
16 1:4 140 20.74 ± 0.94J ND 0.044 ± 0.005K 8.06 ± 0.71J ND ND

SDP, spray-dried particle; ND, not determined.

Means with same letter in the same column (A–K) are not significantly different (p < 0.05).
a
Reported values are the means ± S.D. (n = 3).

625
626 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632
2.6. Total phenolic content
The total phenolic content (TPC) was determined according
to the Folin Ciocalteau method (Slinkard and Singleton, 1977)
with slight modifications. Briefly, samples in methanol solu-
tions were prepared by dissolving 10 mg of spray-dried powder
in 30 ml of methanol and centrifuging for 10 min using a Sar-
torius Sigma 3-18 K centrifuge. The supernatant of the sample
extract (0.5 ml) was added to 2.5 ml of the 0.2 N FC reagent and
allowed to react for 5 min. Then, 2 ml of 75 g/l sodium carbon-
ate was added to the reaction mixture and diluted to 25 ml
using distilled water. Finally, the reaction mixture was incu-
bated for 2 h at room temperature, and the absorbance was
measured at 760 nm using a 4802 UV-VIS double-beam spec-
trophotometer. Methanol was used as the reference. Tannic
acid (0–100 mg/l) was used to produce a standard calibration
curve. The total phenolic content was expressed in mg of tan-
nic acid equivalents (TAE/g of spray-dried powder).
2.7. Total flavonoid content
The total flavonoid content was determined using the Dowd
method as adopted by Arvouet-Grand et al. (1994). A total
of 5 ml of 2% aluminium trichloride (AlCl3 ) in methanol
was mixed with the same volume of the extract solution
(0.4 mg/ml). Absorption readings at 415 nm using a UV-VIS
double-beam spectrophotometer were taken after 10 min
against a blank sample consisting of a 5-ml extract solution
with 5 ml of methanol without AlCl3 . The total flavonoid con-
tent was determined using a standard curve with catechin
(0–100 mg/l) as the standard. The content is expressed as mg
of catechin equivalents (CE/g of extract).
2.8. Moisture content
The moisture content of the spray-dried microparticles was
determined by the oven drying method. Samples of the
microparticles with predetermined masses were placed in an
oven (Memmert), heated to 102 ◦ C and weighed on an analyti-
cal balance (Mettler Toledo PB153-S/FACT, Switzerland) until
a constant mass was observed. The product moisture con-
tent was determined from the weight loss by averaging three
measurements.
2.9. Particle size analyser
The particle size of the spray-dried powder was determined
using a laser scattering particle size distribution analyser
(Horiba LA-300, Japan). Particle size distribution curve was
obtained using software and mean, median, mode, variance
and standard deviation of particle size diameter readings were
also obtained. The measurements were made in triplicate.
2.10. Scanning electron microscopy
The morphology of the spray-dried particles was visualised
using scanning electron microscopy (SEM) (JEOL JSM-5610LV,
Japan) at 10 kV with a magnification of 3000×. Samples were
mounted on self-adhesive carbon sticky tape and gold coated
before imaging (JFC-1600 auto fine coater operated at 20 mA
for 120 s, Japan).
2.11. Fourier transform infrared spectroscopy
The molecular structure changes in raw M. citrifolia L., M.
citrifolia L. extract, spray-dried microparticle powder (1:2 at
90 ◦ C using maltodextrin) and pure maltodextrin were char-
acterised by FTIR analysis. IR spectra were obtained with a
Spectrum 100 series FTIR spectrometer (Perkin Elmer) using
a transformation of 20 scans with a spectral resolution of
4 cm−1 . FTIR spectra were collected in the mid-infrared region
between 4000 and 650 cm−1 . Spectra were acquired using an
air-background correction, and the same spectra were also
obtained using the software.
2.12. Statistical analysis
All experiments were conducted in triplicate and statistical
analysis was done according to SPSS 17.0 software pro-
gram. Analysis of variance was performed by the one-way
ANOVA procedure. Duncan’s multiple range tests were used
to determine significant differences between the means. Mean
differences were considered significant at the p < 0.05 level.
3. Results and discussion
3.1. Spray-dried microparticles of M. citrifolia L. fruit
extract
When the drying time is longer, an accumulation of under-
dried larger particles on the chamber wall may occur, which
leads to low EY values. Thus, the optimal pump flow rate was
fixed. When the inlet air temperature was high, the outlet air
temperature was high, which caused significant particle accu-
mulation on the chamber wall and low EY values. During the
spray-drying process, the spray gas flow rate has little effect
on the product properties. If the feed solution rate is high,
the water will not vaporise fully in the short time allotted,
and the spray-dried powder cannot dry sufficiently. Thus, the
pump rate was fixed as mentioned in Section 2. If the inlet
air temperature is low, there will not be enough heat to dry
the product, and thus, some water will remain in the product.
Wet powders easily stick to the chamber wall (generally, only
powders collected in the container are regarded as effective)
and decrease the EY. Therefore, the lowest inlet air tempera-
ture employed in this study was 90 ◦ C, which is also above the
boiling point (77.1 ◦ C) of the extracted solvent (ethyl acetate).
We found that, at a 1:2 ratio of Mcore /Mwall (␬-carrageenan),
the EY was higher at a lower inlet air temperature (90 ◦ C) than
at higher inlet air temperature (100, 120 and 140 ◦ C) (Table 1
and Fig. 1). This may be due to the volatilisation of active com-
ponents at the higher inlet air temperatures. Even at 90 ◦ C,
the EY was only around 32%. For a 1:2 ratio of Mcore /Mwall
(␬-carrageenan) at 140 ◦ C, most of the particles obtained by
spray-drying accumulated on the chamber wall, and hence,
the EY was only approximately 8%. This may be due to low
moisture content of particles which tend to deposit on the
chamber wall. At the 1:1 ratio of Mcore /Mwall (␬-carrageenan),
the EY was higher at 140 ◦ C than at the other inlet air tem-
peratures. At 90 and 100 ◦ C, for the same ratio, the EY was
at its minimum, and little ethyl acetate was observed in the
liquid collector. It may be that the 1:1 ratio is not an appro-
priate proportion because it lacks a sufficient amount of the
binding material. At the 1:1 ratio at 120 ◦ C, even though the
EY was minimal, there was no observed ethyl acetate extract
 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632 627

(a) 30
Table 3 – DPPH scavenging activity of Morinda citrifolia L.
fruit.
25
DPPH activity (%)

S. no. Sample DPPH scavenging

20 activity (%)a

1 Fruit extract 75.92 ± 0.88B

15
2 Concentrated fruit extract 45.00 ± 1.24C
3 BHT 80.12 ± 0.76A
10
4 ␣-Tocopherol 74.25 ± 0.97B
5
Means with same letter (A–C) are not significantly different
(p < 0.05).
0
90 100 120 140
a
Reported values are the means ± S.D. (n = 3).
Temperature (deg C)
1:1 Mcore/Mwall 1:2 Mcore/Mwall 1:4 Mcore/Mwall 1:6 Mcore/Mwall

suggested before, this may be caused by an increase in the

(b) 35 amount of active components volatilization or deterioration.
30 However, at 1:1 ratio and inlet air temperatures (90–100 ◦ C),
the DPPH was found to be 15.85% and 11% respectively which
DPPH activity (%)

25
20
15
10
5 the 1:2 ratio of Mcore /Mwall at 90 ◦ C exhibited 24.91% DPPH scav-
0
90 100 120
Temperature (deg C)
1:1 Mcore/Mwall 1:2 Mcore/Mwall 1:3 Mcore/Mwall
Fig. 1 – Percentage of DPPH scavenging activity of
spray-dried Morinda citrifolia L. fruit extract with respect to
temperature for (a) ␬-carrageenan and (b) maltodextrin
(with error bars).
in the liquid collector. This may be attributable to active com-
ponent volatilisation or wall binding. Similarly, at the 1:1 ratio
at 140 ◦ C, there was no observed ethyl acetate extract in the
liquid collector. At the 1:6 and 1:4 ratios of Mcore /Mwall (␬-
carrageenan), the highest EYs were obtained at 90 and 100 ◦ C,
respectively. In general, when compared to all other condi-
tions, the EY was found to be highest for the 1:1 ratio of
Mcore /Mwall at 140 ◦ C for the spray-dried M. citrifolia L. fruit
extract with ␬-carrageenan as the binding material. However,
at this ratio (1:1 at 140 ◦ C), the DPPH scavenging activity was
found to be lower.
At the 1:2 ratio of Mcore /Mwall (maltodextrin), the EY was
higher at a higher inlet air temperature (140 ◦ C) than at lower
inlet air temperatures (90, 100 and 120 ◦ C) (Table 2 and Fig. 2).
This may result from the active components effectively attach-
ing to the binders. In general, when compared to all other
conditions, the EY observed for the 1:2 ratio at 140 ◦ C was
a maximum (39.16%) for the spray-dried M. citrifolia L. fruit
extract with maltodextrin as the binding material. However,
some researchers have obtained a higher EY; for example, in
the microencapsulation of Radix salvia miltiorrhiza, EY values of
52.96–62.73% have been obtained (Su et al., 2008). Conversely,
we found that the EY values are consistent for a similar set of
parameters (operating conditions).
3.2. DPPH, total phenolics and total flavonoids
As the inlet air temperature increased from 90 to 140 ◦ C at
all ratios (1:1, 1;2, 1:4 and 1:6) of Mcore /Mwall (␬-carrageenan),
the percentage of DPPH scavenging activity decreased. As
are low compared to other ratios at this inlet air temperatures
due to presence of ethyl acetate in the liquid collector. This
study found that, at the 1:6 ratio of Mcore /Mwall at 90 ◦ C, the
percentage of DPPH scavenging activity was 25.32%, which is
the highest when compared to all of the other ratios. However,
enging activity (Table 1). Because there is not much difference
140
in the percentage of DPPH scavenging activity, we suggest the
use of the 1:2 ratio at 90 ◦ C because, at this ratio, the amounts
of non-active components (the excipients) are smaller and the
1:4 Mcore/Mwall
EY is maximised. However, the EY for 1:2 at 90 ◦ C is only 31.56%.
As the inlet air temperature increased for a 1:2 ratio of
Mcore /Mwall (maltodextrin), the percentage of DPPH scaveng-
ing activity decreased (Table 2). As the inlet air temperature
increased for the 1:1 and 1:4 ratios of Mcore /Mwall (mal-
todextrin), the percentage of DPPH scavenging activity also
decreased; this may be due to the volatility of bioactive compo-
nents or component deterioration. This study also found that,
for the 1:2 ratio of Mcore /Mwall (maltodextrin concentration,
33 mg/ml) at 90 ◦ C, the percentage of DPPH scavenging activ-
ity was 28.36%, which is the highest of all of the ratios. This
is due to a smaller volatility loss of the bioactive components
and the appropriate amount of binding material added for this
operating condition. The DPPH scavenging activity of the ethyl
acetate M. citrifolia L. fruit extract is approximately 76%, which
is similar to the DPPH scavenging activity of BHT (80.12%)
(Table 3). And there is no significant difference between fruit
extract and ␣-tocopherol (p < 0.05). These results are consis-
tent with other findings (Mohd Zin et al., 2002, 2006).
However concentrated fruit extract showed DPPH scav-
enging activity 45% only. This is because of volatilization of
bioactive components in the rotary evaporator due to temper-
ature effect. The DPPH scavenging-activity of the encapsulated
powders, regardless of process conditions, decreased signifi-
cantly with respect to the fresh fruit extract, due to the spray
drying process (compare results from Tables 1 and 2 with
Table 3); i.e., from 76% fresh fruit extract down to 28% encap-
sulated powder at optimal condition. This is in agreement
with results found by Yang et al. (2007) who reported a lost
of 65% radical scavenging activity due to heating between 65
and 75 ◦ C.
Samples that exhibited higher percentages of DPPH scav-
enging activity were selected for TPC analysis. Although the
FC procedure does not give a full picture of the quantity and
quality of the phenolic constituents of the extracts, this widely
used method provides a rapid and useful overall evaluation
628 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632

(a) 40

35

Total phenolic content

30

(mg of TAE/g of SDP)

25

20

15

10

0
90 100 120
Temperature (deg C)

1:1 Mcore/Mwall 1:2 Mcore/Mwall 1:4 Mcore/Mwall 1:6 Mcore/Mwall

(b) 60

50
Total phenolic content
(mg of TAE/g of SDP)

40

30

20

10

0
90 100 120
Temperature (deg C)

1:1 Mcore/Mwall 1:2 Mcore/Mwall 1:3 Mcore/Mwall 1:4Mcore/Mwall

Fig. 2 – Total phenolic content of spray-dried powder at different temperatures for different ratios of Mcore /Mwall : (a)
␬-carrageenan, (b) maltodextrin (with error bars).

of the phenolic content of extracts. As with the percent-
age of DPPH scavenging activity, the TPC was also higher for
the 1:6 ratio at 90 ◦ C (␬-carrageenan) at 36 mg of TAE/g of
spray-dried powder. However, for the 1:2 ratio of Mcore /Mwall
(␬-carrageenan) at 90 ◦ C, the TPC was also found to be 36 mg of
TAE/g of spray-dried powder. With maltodextrin as the binding
material, the TPC was highest (54 mg of TAE/g of spray-dried
powder) at 1:2, 90 ◦ C.
As before, the samples that exhibited the highest percent-
age of DPPH scavenging activity and TPC were selected for total
flavonoid analysis. The TF was also higher for the 1:6 ratio of
Mcore /Mwall at 90 ◦ C at 30 mg of CE/g of SDP for ␬-carrageenan.
However, for the 1:2 ratio of Mcore /Mwall (␬-carrageenan) at
90 ◦ C, the TF was also found to be 30 mg of CE/g of SDP. When
maltodextrin was used as the binding material, the TF was
highest (45 mg of CE/g of spray-dried powder) at a ratio of 1:2
at 90 ◦ C (Table 2).
3.3. Moisture content
The results showed that at a constant feed flow rate, the
moisture content of the spray-dried powders decreased with
increasing inlet and outlet air temperature for ␬-carrageenan
and maltodextrin (Tables 1 and 2). This is because at higher
inlet air temperatures, the rate of heat transfer to the particle
is greater, providing a greater driving force for moisture evapo-
ration. Consequently, powders with reduced moisture content
are formed. These results are consistent with other findings
(Goula et al., 2004; Quek et al., 2007).
The moisture content of the spray-dried powder decreased
when the amount of maltodextrin added increased (Table 2).
In a spray-drying system, the water content of the feed
has an effect on the final moisture content of the powder
produced (Abadio et al., 2004). The addition of maltodextrin to
the feed prior to spray-drying increased the total solid content
and reduced the amount of water available for evaporation.
Hence, a decrease in the moisture content of the powder
was observed. This means that powders with lower moisture
contents can be obtained by increasing the percentage of mal-
todextrin added. However, if the percentage of maltodextrin
is too high, the powder produced will have a lower quality
because the chemical components from the M. citrifolia L. juice
will be diluted. These results are also consistent with other
findings (Quek et al., 2007).
3.4. Appearance and particle size
Electron micrographs of M. citrifolia L. spray-dried under dif-
ferent operating conditions (Fig. 3) confirmed that the particle
powders were micron-sized (2–5 ␮m, mean diameter). Most of
the particles had spherical shapes and showed little agglom-
eration. All of the spray-dried microcapsules containing
␬-carrageenan and maltodextrin with different antioxidant
equivalents appeared to be smooth spheres. The presence of
coating agents, such as ␬-carrageenan or maltodextrin, that
react as plasticisers is important for promoting the forma-
tion of spherical and smooth-surfaced microparticles (Bruschi
et al., 2003). Similar smooth spheres have primarily been
observed in microcapsules of black carrot pigments (Daucus-
carota L.) with maltodextrin (10DE and 20-23DE) (Ersus and
Yurdagel, 2007).
The microparticle size of the spray-dried M. citrifolia L. fruit
extract for the 1:2 ratio of Mcore /Mwall at 90 ◦ C was found to be
2.27 ␮m and 4.82 ␮m (mean diameter) for ␬-carrageenan and
maltodextrin, respectively, with a particle size analyzer and a
typical particle size distribution curve is shown in Fig. 4. This
 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632 629

Fig. 3 – SEM of spray-dried powders of M. citrifolia L. achieved using ␬-carrageenan (a–c) and maltodextrin (d–f) as the wall
material under the following conditions: (a) 1:2 at 90 ◦ C, (b) 1:6 at 90 ◦ C, (c) 1:6 at 100 ◦ C, (d) 1:2 at 90 ◦ C, (e) 1:4 at 120 ◦ C and (f)
1:4 at 140 ◦ C.

Fig. 4 – Particle size distribution curve of spray-dried powder of 1:2 at 90 ◦ C (␬-carrageenan).

increase in particle size is related to the molecule size of each
carrier agent (Tonon et al., 2010). In general, all of the tested
samples exhibited a similar particle size distribution, regard-
less of the inlet air temperature or the ratio of Mcore /Mwall .
However, an analysis of the particle size distribution revealed
that at the optimal operating condition for ␬-carrageenan, the
mean particle size diameter was slightly lower when com-
pared to the other ratios (Fig. 5).
in the extract (Djeridane et al., 2006). For this reason, samples
with similar total phenolic contents may vary in their scav-
enging activity. A further relationship between DPPH and the
total phenolic content (TPC) was found to be:
0.751
DPPH = 1.465 (TPC) (1)

3.5. Correlation of DPPH with total phenolics and total

flavonoids

The experimental values of the percentage of DPPH scav-

enging activity of M. citrifolia L. microparticles were fitted as
a function of the total phenolic content to detect any rela-
tionships among the antioxidant activities of the phenolic
compounds. The correlation coefficient between the DPPH
scavenging activity and the total phenolic content of the M.
citrifolia L. microparticles is 0.85. This result suggests that
approximately 85% of the antioxidant capacity of the spray-
dried M. citrifolia L. fruit extract may be attributed to the Fig. 5 – Particle size analysis of spray-dried powder at 90 ◦ C
contribution of phenolic compounds. In fact, the total pheno- for different ratios of Mcore /Mwall : (a) ␬-carrageenan and (b)
lic content does not encompass all of the antioxidants present maltodextrin (with error bars).
630 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632

Similarly, a positive correlation was found between DPPH

scavenging activity and total flavonoid content as:

0.735
DPPH = 1.565 (TF) (2)

By combining Eqs. (1) and (2), the correlation between the

variables was found to be:

0.751 0.735
DPPH = 0.057 (TPC) (TF) (3)

The average deviation between the experimental and cal-

culated DPPH values was found to be 12.5% and 9.4% for
␬-carrageenan and maltodextrin, respectively (Fig. 6).

3.6. FTIR analysis

FTIR analysis provides information about chemical bonds and

the molecular structure of materials. The FTIR spectra of M.
citrifolia L. raw powder, extract and spray-dried powder (using
maltodextrin) and pure maltodextrin were recorded (individ-
ual datasets not shown). The FTIR spectra of all of the above
were compared and are shown in Fig. 7.
The spectrum of raw powder shows the band at 3365,
2925, 1627, 1417, 1251, 1035 and 773 cm−1 . Band at 3365 cm−1
due to O–H stretching (3200–3550 cm−1 ), 2925 due to sp3 C–H
stretching (2850–3000 cm−1 ), 1627 assigned to C O stretch- Fig. 6 – Correlation between percentage of DPPH
ing (amides, 1630–1695 and esters 1735–1750 cm−1 ). Since N–H scavenging activity of spray-dried Morinda citrifolia L. fruit
spike was not found it represents absence of amides. 1417 due extract with (a) total phenolic content and (b) total flavonoid
to ␣-CH2 bending (1400–1450 cm−1 ), 1251 and 1035 due to C–O (for both additives).
stretching (1000–1300 cm−1 ), 773 assigned to C–H bending and
ring puckering (690–900 cm−1 ). Most of these observations are stretching, band at 937 assigned to CH and CH2 bending
similar with Wang et al. (1999) work for the compound isolated (880–995 cm−1 ), 846 and 787 due to CH bending and ring puck-
from fruit extract of M. citrifolia L. ering. The intensity of the band at 1742 is high due to presence
The spectrum of fruit extract shows the band at 2984, 1742, of ethyl acetate in the conventional extract and due to car-
1447, 1376, 1239, 1098, 1048, 937, 846 and 787 cm−1 . Band at bonyl group of aromatic acids. The absence of O–H stretching
2984 cm−1 due to sp3 C–H stretching, 1742 due to C O stretch- was found in the extract whereas high intensity of peak was
ing esters, 1447 assigned to ␣-CH2 bending. 1376 due to O–H seen in M. citrifolia L. raw powder. However O–H bending
bending (1330–1430), 1239, 1098 and 1048 assigned to C–O was observed in the extract with high intensity as well. This
%T

4000.0 3600 3200 2800 2400 2000 1800 1600 1400 1200 1000 800 650.0
cm-1

Fig. 7 – Raw powder (blue), extract of hot water extraction (green), 1:2 at 90 ◦ C maltodextrin (red), pure maltodextrin (pink).
(For interpretation of the references to color in this figure legend, the reader is referred to the web version of the article.)
 chemical engineering research and design 9 0 ( 2 0 1 2 ) 622–632
indicates all the phenols and carboxylic acids and derivatives
have been extracted from the M. citrifolia L. raw powder effec-
tively.
The spectrum of pure maltodextrin shows the band at 3345,
2936, 1647, 1413, 1370, 1150, 1076, 931, 854, and 761 cm−1 . The
characteristic peak at 3345 cm−1 due to O–H stretching, 2936
due to sp3 C–H stretching, 1647 assigned to C O stretching and
1413 due to ␣-CH2 bending, 1370 due to O–H bending, 1150 and
1076 due to C–O stretching, 931 due to CH and CH2 bending
and 854 and 761 due to C–H bending and ring puckering.
The spectrum of spray dried powder (1:2 at 90 ◦ C) shows
the band at 3345, 2936, 1740, 1362, 1152, 1076, 1021, 930, 848
and 763 cm−1 . The characteristic peak at 3345 cm−1 due to O–H
stretching, 2936 due to sp3 C–H stretching and 1740 assigned to
C O stretching esters. The peak corresponds to O–H stretching
was found here, this may be due to presence of wall material,
maltodextrin. The intensity of peak at 1740 is low; it indicates
the evaporation of ethyl acetate in the spray dried powder.
Very weak C O stretching band which was found in maltodex-
trin not appeared in the spray dried sample. And also ␣-CH2
bending disappeared in the spray dried sample which was
found in raw powder and extract. This is due to volatiliza-
tion of bioactive components in the spray dried powder. These
results are consistent with the DPPH assay. All the other peaks
appeared in M. citrifolia L. raw powder and maltodextrin also
appeared in microencapsulated powder, indicating that no
chemical interaction between bioactive component of fruit
extract and wall material (Fig. 7).
No molecular structure change observed between the
raw powder, the spray-dried powder and pure maltodextrin,
because the characteristic peaks did not show any shifts,
except for the spectrum of M. citrifolia L. extract. This shows
that the active ingredients of M. citrifolia L. were retained after
spray-drying using maltodextrin.
4. Conclusions
For extracts containing volatile components, temperature is
one of the most important factors during food processing as
well as in sample handling and storage. The effect of inlet
air temperature on the water activity of a dried product is
also very important, but not fully understood. The results of
this study show that the highest antioxidant activity, total
phenolic content and total flavonoid content were found at
a 1:2 ratio of Mcore /Mwall at 90 ◦ C for maltodextrin. Under
these optimal operating conditions, the antioxidant activity,
total phenolic content and total flavonoid content were found
to be 28.36%, 54 mg of TAE/g of SDP and 45 mg of CE/g of
SDP, respectively. The encapsulation yield, particle size and
moisture content of the spray-dried fruit extract produced
using maltodextrin as the adjuvant were found to be 27.64%,
4.82 ␮m and 13.3%, respectively. In addition, the M. citrifolia L.
microparticles obtained in this work showed valuable antiox-
idant activity, suggesting their possible use as a natural and
multifunctional dietary food additive or supplement. Because
the pharmaceutical value of this fruit is very high, it is impor-
tant to identify the nutritional and functional compounds that
it contains and to explain their mechanisms of action. In this
way, we can assess the real potential of this fruit and the tech-
nological processes necessary to preserve the fruit’s beneficial
properties.
The antioxidant activities of the spray-dried M. citrifolia L.
fruit extract were affected by the spray-drying temperature.
It was found that ␬-carrageenan and maltodextrin are both
631
effective drying aids for the spray-drying of M. citrifolia L. fruit
extract. However, maltodextrin can be used preferentially over
␬-carrageenan.
Acknowledgements
The authors wish to acknowledge the financial support of
MOSTI Malaysia. This work was carried out under an e-science
grant, number SCF0049-IND-2007.
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