JFS: Food Chemistry and Toxicology

Characteristics of Double-Encapsulated
Flavor Powder Prepared by
Secondary Fat Coating Process
Y.H. CHO AND J. PARK
Food Chemistry and Toxicology

ABSTRACT: Double encapsulation of single-encapsulated powder containing flavor compounds was performed by
a fat coating process using molten hydrogenated palm kernel oil (melting point = 47.3 °C). Double-encapsulated
powder showed a 47% increase in mean particle size and a 33% reduction in moisture uptake. Single-encapsulated
powder exhibited rapid limonene oxidation throughout the storage time, while double-encapsulated powder was
consistently stable. SEM images of the double-encapsulated powder showed singular or aggregated particles covered
with a continuous fat matrix. Thermally controlled release from the double-encapsulated powder was observed.
Flavor release from the double-encapsulated powder ranged from 36.6% to 57.8% at 37 °C, with an increase to 81.3
to 95.0% at 60 °C.
Keywords: double encapsulation, fat coating, flavor, controlled release

Introduction vors for chewing gum. Li and Reineccius (1995) described a sec-

E NCAPSULATION HAS BEEN USED : (1) TO PROTECT FLAVOR FROM

oxidation caused by heat, light, humidity, and other sub-
stances over a long shelf life; (2) to prevent evaporation of vola-
tile components; and (3) to convert flavor in liquid form to solid
form (Kenyon and Anderson 1988; Shahidi and Han 1993). Hy-
drocolloids, such as starch, dextrin, maltodextrin, gum arabic,
and gelatin are commonly used as wall materials. Products of this
type used in encapsulation retain a good flavor profile and are
easy to handle. However, they are water-soluble, suffer from fla-
vor loss under long-term storage, and may release flavor too rap-
idly in some applications (Sparks and others 1995). To solve
these problems, it has been customary to coat spray-dried pow-
der, or some other solid form of the flavor, with fat or wax. The fat
coating is commonly performed using a fluidized bed coating or
spray chilling. When spray-dried powder is used as the core ma-
terial, the process is called double encapsulation (Tan 1991). The
coating must be applied as a film with a uniform thickness suffi-
cient to provide a barrier against degradative factors such as
moisture, pH change, temperature change, and reactive chemi-
cals (Churukuri 1990).
In some cases, melting of the coating material can be used as
a release method. Thermally controlled release of flavor com-
pounds is a characteristic property of secondary fat coated flavor
powder (Li and Reineccius 1995). Controlled release is a novel
technology that can be used to increase the effectiveness of
many ingredients and is defined as a method by which 1 or more
active agents or ingredients are made available at a desired site,
at a specific time, and at a specific rate. With the emergence of
controlled-release technology, heat-, temperature-, or pH-sensi-
tive additives can be conveniently used in food systems (Po-
thakamury and Barbosa-Canovas 1995).
Many patents relating to the multiple encapsulation system
using hydrogenated oil and waxes have been granted (Zibell
1989; Cherukuri and others 1990, 1991; Tan and others 1991;
King and others 1996). The major area of application for these
patents is sustained or controlled release of sweeteners and fla-
ondary fat coating process for use as an ingredient in microwave
frozen pancakes. However, no published research has referred to
the physical properties and structures of double-encapsulated
powders. Onwulata and others (1998) investigated the character-
istics of double-encapsulated powder containing anhydrous
butter oil, but lacking flavor compounds.
The objectives of this study were to investigate the physical
properties and microstructure of double-encapsulated powder
containing flavor compounds, leading to a comparison with the
single-encapsulated powder, and to observe the characteristics
of melting-activated flavor release from double-encapsulated
powder.
Materials and Methods
Flavor model system
Five flavor compounds were selected based on boiling points
(90 to 200 °C) and molecular weights (MW 100 to 140 Da). These
compounds were ethyl propionate, butyl acetate, 2-heptanone,
limonene, and octanol-1. All were purchased from Sigma Co. (St.
Louis, Mo., U.S.A.). These flavor components were mixed with
rapeseed oil (1 part flavor: 4 parts oil).
Wall materials
The carbohydrate wall system consisted of a mixture of malto-
dextrin (DE = 15, Sewon Co., Seoul, Korea), gum arabic ( TIC
Gums, Belcamp, Md., U.S.A.), N-Lok (National Starch and Chem-
ical Co., Bridgewater, N.J.,U.S.A.), and gellan gum (Kelco, SAN
DIEGO, CALIF., U.S.A.) at a ratio of 30 : 26.4 : 39.6 : 4 (Cho and
others 1999). Hydrogenated palm kernel oil (melting point =
47.3 °C) was used as a coating fat.
Emulsion and microcapsule preparation
Wall material was weighed and reconstituted in distilled water
at a 30% w/v concentration using a homomixer (Model 2.5 spec,
Tokushu Kikka, CITY?Japan). The coarse emulsion was prepared

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 Characteristics of double-encapsulated flavor powder . . .
by blending the core/wall (1:4) mixture for 10 min at 10,000 rpm
with a homomixer. The mixture was then homogenized at 20 MPa
using a piston-type homogenizer (Rannie, APV, Albertslund,
Denmark). This emulsion was spray-dried in a disk-type spray
dryer (L-8, Ohkawara Kakohki, Yokohama, Japan) at an air inlet
temperature of 180 °C (outlet temperature = 100 °C) and a nozzle
speed of 15,000 ± 100 rpm. Double-encapsulated powder was
prepared from single-encapsulated powder by the secondary fat
coating process. The hydrogenated palm kernel oil was melted at
50 °C. Single-encapsulated powder prepared as above was put
into the coating chamber of a flow coater (Cheil Mechanical Co.,
Seoul, Korea). Molten hydrogenated palm kernel oil was atom-
ized through nozzles into the chamber, while single-encapsulat-
ed powders were suspended in upward-moving stream of air.
The double-encapsulated powder coated with hydrogenated oil
was hardened by cool air.
Total oil determination
The total oil content of the single-encapsulated powder was
determined using a Clevenger trap (Reineccius and others 1995).
Single-encapsulated powder (30 g) was dispersed in 200 mL of
distilled water in 500 mL flat-bottomed flask. The Clevenger trap
and a water-cooled condenser were fitted into the top of the boil-
ing flask and distilled for 2 h. The volume of oil collected in the
trap was directly read from oil collecting arm of the Clevenger ap-
paratus and multiplied by a density factor of 0.9 g/mL to calcu-
late the weight of oil recovered from the sample.
Surface oil determination
The surface oil content of the single-encapsulated powder
was determined using a Soxhlet extraction apparatus according
to the method of Reineccius and others (1995). A Hewlett Pack-
ard 6890 gas chromatograph equipped with a flame ionization
detector was used for detection. Separation was achieved on a 25
m × 0.32 mm I.D. × 0.17 µm Ultra II column (Hewlett-Packard,
Wilmington, Del., U.S.A.). The oven temperature was held at
35 °C for 5 min, and then increased at 10 °C/min to 180 °C. The
injection port and detector were maintained at 200 and 250 °C,
respectively. Hydrogen was used as a carrier gas at a column flow
rate of 1 mL/min. Each flavor compound (0.2 mL) was mixed with
Figure 1—Particle size distribution of encapsulated flavor
powders. 䊊: single-encapsulated powder, 䉭: double-encap-
sulated powder.
jfsv67n3p0968-0972ms20010160-MO-wcxs.p65969
200 mL of pentane in a 500 mL flask and evaporated as above, for
use as an external standard.
Determination of the amount of coating fat
The extractable fat content of double-encapsulated powder
was determined according to the method of Li and Reineccius
(1995). Double-encapsulated powder (2 g) was placed in an ex-
traction thimble. The thimble containing powder was weighed.
Extraction was done in a Soxhlet extractor with petroleum ether
(150 mL) for 3 h. The thimble was dried in an air-drying oven at
80 °C for 1 h. The thimble and its contents were weighed to calcu-
late the fat content and the percent fat in the powder was calcu-
lated.
Food Chemistry and Toxicology
Moisture content
The AOAC (32.1.03., 1995) method for flour was used for mois-
ture determination. All samples were analyzed in duplicate.
Moisture uptake
Each powder was placed in a petri dish and weighed. The
moisture uptake of the powder was determined at 25 °C and 80%
relative humidity in an incubator (KCL-1000, Eyela, Tokyo, Ja-
pan). Measurements were carried out in duplicate.
Particle size
Single-encapsulated powder was dispersed in ethanol. The
particle distribution and mean particle size were analyzed using
a particle size analyzer (Analysette 22, Fritsch, Idar–Oberstein,
Germany). Double-encapsulated powders were dispersed in dis-
tilled water and analyzed as above. Measurements were made in
triplicate.
Microstructural properties
Scanning electron microscopy (S-4200, Hitachi, Tokyo, Japan)
was used to investigate the microstructural properties of single-
and double-encapsulated powders. Microencapsulated speci-
mens were loaded onto a specimen stub with two-sided adhesive
tape. Specimens were subsequently coated with gold by ion
sputter (␧–1030, Hitachi). For study of internal particle structure,
encapsulated powders were frozen at –20 °C for 1 h, then broken
Figure 2—Moisture uptake of single- and double-encapsu-
lated powders at 25 °C, 80% RH. 䉭: single-encapsulated
flavor powder, 䊊: double-encapsulated flavor powder.
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 Characteristics of double-encapsulated flavor powder . . .

Table 1 ¯ Composition and properties of single- and double- in the mean particle size in the double-encapsulated powder.
encapsulated powders The single-encapsulated powder had a narrower particle size
Single- Double- range with a relatively uniform distribution, while the double-
Total oil retention (%) 61.3 nm encapsulated powder showed a broader size range. These results
Surface oil content (mg/100g) 5.12 nm agree with Onwulata and others (1998). The larger particle size of
Coating amount (%) nm 31.5 double-encapsulated powder is due to the aggregation of single-
Moisture content (%) 1.20 1.80 encapsulated powder grains within the fat matrix. Smaller parti-
Particle size mean (µm) 30.7 45.2
cles may be a fragment of fat.
Particle size range (µm) 15.2 - 43.5 0.67 - 94.4
The moisture uptake rate of encapsulated powders (Figure 2)
nm: not measured.
increased rapidly, and then remained constant. Double-encap-
sulated powder absorbed much less moisture than single-encap-
sulated powder. Double-encapsulated powder is more efficient
as a moisture barrier and for moisture sorption. This functional-
Food Chemistry and Toxicology

with tweezers.
Oxidative stability
Each microencapsulated powder was stored in an incubator
at 37 °C. Every 7 d, 0.3 g of powder was withdrawn and dissolved
in 10 mL of HPLC grade water in a 50 mL centrifuge tube. The
centrifuge tubes were sealed and shaken vigorously for 1 min us-
ing a vortex mixer. The tubes were then stored at 60 °C for 1 h.
HPLC grade pentane (5 g) containing 1 mg of nonane as an inter-
nal standard was added to each tube, then the tubes were shak-
en as before. The tubes were transferred to a shaking incubator
and maintained at 40 °C for 1 h, then centrifuged for 10 min at
3000 × g (Union 55R, Hanil Co., Inchon, Korea). The clear super-
natant layer (1 ␮L) was analyzed by GC for determination of the
surface oil. The formation of limonene 1,2-epoxide from L-limone
during 37 °C storage was measured as an indicator of oxidative
stability in the single- and double-encapsulated powders.
Determination of flavor release from double-
encapsulated powder
A manual solid phase microextraction (SPME) fiber holder
and a 100 ␮m polydimethylsiloxane coated fiber were used (Su-
pelco, Bellefonte, Pa., U.S.A.). Sample (1.5 g) was weighed into a
50-mL headspace vial and 28.5 mL of distilled water was added.
The vial was sealed with a Teflon-coated septa and an aluminum
cap. The samples incubated at 37 °C for 1 h and 60 °C for 1 h be-
fore analysis. The vial was immersed in a 30 °C water bath. An
SPME needle was inserted through the septum and the SPME fi-
ber was allowed to equilibrate for 15 min with sonication. The
SPME fiber was exposed in the GC inlet (250 °C) for 15 s during
the desorption step.
ity enhances the benefits of encapsulation for storage stability
against moisture and light.
Oxidative stability
Limonene was selected from among several flavor com-
pounds to use as an indicator of oxidative stability. Limonene is 1
of the most abundant hydrocarbons found in essential oils, but
its main drawback is a tendency to oxidize (Arctander 1969).
When orange peel oil is stored at elevated temperature the 2
oxidation products of limonene, limonene-1, 2-epoxide and car-
vone appear during storage. Since limonene-1, 2-epoxide and
carvone are the earliest compounds observed during oxidation,
they were used as indicators of oil oxidation (Anandaraman and
Reineccius 1986). The results of limonene oxide formation for
single- and double-encapsulated powders observed up to 20 wk
at 37 °C are shown in Figure 3. Single-encapsulated powder ex-
hibited limonene-1, 2-epoxide formation after 7 wk. The forma-
tion rate of limonene oxidation in single-encapsulated powder
was much faster than for double-encapsulated powder. Similar
results were observed for the formation of carvone during stor-
age, although with a lesser amount and a slower formation rate
(data not shown). The rate of limonene oxidation is a function of
several factors, including water activity, availability of oxygen,

Results and Discussion

Composition and properties of single- and double-

encapsulated powders
The measured composition and properties of single- and dou-
ble-encapsulated powders are shown in Table 1. The total oil re-
tention and surface oil content of single-encapsulated powder
were 61.3% and 5.12 mg/100 g, respectively. The amount of coat-
ing fat of double-encapsulated powder was 31.5%. Moisture
analysis results showed that the percent moisture content in sin-
gle-encapsulated powder remained approximately 1%. Double-
encapsulated powder had higher moisture content, which may
be due to the absorption of moisture from the environment dur-
ing secondary fat coating process. Onwulata and others (1998)
also observed higher moisture content in the double-encapsu-
Figure 3—Changes in concentration of limonene 1,2-ep-
lated powder. The particle size distribution of double-encapsu- oxide formed from encapsulated flavor powders during
lated powder was measured and compared to the distribution of storage at 37 °C. 䉭: single-encapsulated flavor powder, 䊊:
single-encapsulated powder (Figure 1). There was a 47% increase double-encapsulated flavor powder.

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 Characteristics of double-encapsulated flavor powder . . .
Figure 4—SEM micrograph of encapsulated flavor powder.
A: single-encapsulated flavor powder at 200×, B: double-
encapsulated flavor powder at 100×.
Figure 5—A high magnification SEM micrograph of double-
encapsulated flavor powder grains at 2000×.
jfsv67n3p0968-0972ms20010160-MO-wcxs.p65971
Food Chemistry and Toxicology
Figure 6—SEM micrograph of shattered particles. A: single-
encapsulated flavor powder at 2,000×, B: double-encap-
sulated flavor powder at 2,000×.
trace mineral composition, and the presence of antioxidants
(Kim and Morr 1996). The coating of fat acts as a barrier so that
the rate of limonene oxide formation in double-encapsulated
powder is reduced.
Microstructural properties
SEM images of single-encapsulated powder grains showed
relatively spherical and smooth particles (Figure 4A). Formation
of particles with dented surfaces may be due to rapid shrinkage
of the liquid droplets during the early stage of the drying process
(Kim and Morr 1996. Double-encapsulated powder grains were
typically singular or aggregated particles (Figure 4B). A higher
magnification micrograph of double-encapsulated powder
grains shows that a fat matrix was formed around the single-en-
capsulated powder particles (Figure 5). According to Onwulata
and others (1998), double-coated powder can be a simple or
compound powder with more than 1 particle encased within the
fat matrix. This explains the wider particle size distribution for
double-encapsulated powder.
The interior structure of the particle wall in single-encapsulat-
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 Characteristics of double-encapsulated flavor powder . . .
ed powder shows a porous wall of < 6 ␮m thickness (Figure 6A).
Flavor compounds were dispersed in the capsule wall as small
droplets of < 2 ␮m dia. A large void was observed in the center of
the capsule. This typical structure has been observed in spray-
dried microcapsules by several investigators (Rosenberg and
others 1990; Sheu and Rosenberg 1995). Formation of the void is
related to expansion associated with temperature increase with-
in the capsule during the late stages of drying. Fractured parti-
cles of simple, double-encapsulated powders show a porous wall
of thickness < 7.5 ␮m covered by a coating of fat (Figure 6B).
Thermal release
According to Sparks and others (1995), and in agreement with
Food Chemistry and Toxicology
our results, coated particles may be efficiently stored at temper-
atures below the melting point of the coating material, and are
protected from release in water for a certain period of time during
mixing and preparation. However, the flavor can be released dur-
ing cooking. As shown in Figure 6, flavor release from double-en-
capsulated powder ranged from 81.3% to 95.0% when the tem-
perature exceeded the melting point of the coating fat. Flavor
compounds are quickly released when the coating fat melts at a
high temperature and the double-encapsulated powder is dis-
solved in water. However, since the incubation time is too short,
flavor release from the dissolved powder does not reach 100%.
Flavor release is retarded (36.6 to 58.8%) at an incubation tem-
perature lower than the melting point. This result indicated that
the coating was not complete, allowing some of double-encapsu-
lated powder particles to dissolve in water. Consequently the fla-
vor release at 37 °C from double-encapsulated powder was
greater than expected.
Figure 7—Flavor release from double-encapsulated flavor
powder incubated at 37 °C (䊏) and 60 °C (䊐).
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Conclusion
D OUBLE-ENCAPSULATED POWDERS HAVE A HIGHER RESISTANCE TO
moisture and oxygen than single-encapsulated powders, as
particles were encased within the fat matrix. It indicated that a
secondary-fat coating could be used as an effective method for
protecting sensitive ingredients. Melting-activated release from
encapsulated powders was achieved by the secondary-fat coat-
ing process. The melting-activated release system is applicable
in the food industry since many foods such as microwave foods
and hot drinks are heated prior to consumption and thus, ingre-
dients can be protected until their final use.
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MS 20010160 Submitted 3/31/01, Revised 6/18/01, Accepted 6/19/01, Received
1/28/02
Authors are with Dept. of Biotechnology, Yonsei Univ., Seoul 120-749, Korea.
Direct inquiries to author Park (E-mail: foodpro@yonsei.ac.kr).
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