Recent Developments in Microencapsulation of Food Ingredients
Recent Developments in Microencapsulation of Food Ingredients
Recent Developments in Microencapsulation of Food Ingredients
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Dry<strong>in</strong>g Technology, 23: 1361–1394, 2005<br />
Copyright Q 2005 Taylor & Francis, Inc.<br />
ISSN: 0737-3937 pr<strong>in</strong>t/1532-2300 onl<strong>in</strong>e<br />
DOI: 10.1081/DRT-200063478<br />
<strong>Recent</strong> <strong>Developments</strong> <strong>in</strong> <strong>Microencapsulation</strong> <strong>of</strong><br />
<strong>Food</strong> <strong>Ingredients</strong><br />
Kashappa Goud H. Desai and Hyun J<strong>in</strong> Park*<br />
Graduate School <strong>of</strong> Biotechnology, Korea University, Sungbuk-ku,<br />
Seoul, South Korea<br />
Abstract: <strong>Microencapsulation</strong> <strong>in</strong>volves the <strong>in</strong>corporation <strong>of</strong> food <strong>in</strong>gredients,<br />
enzymes, cells, or other materials <strong>in</strong> small capsules. Microcapsules <strong>of</strong>fer food processors<br />
a means with which to protect sensitive food components, ensure aga<strong>in</strong>st<br />
nutritional loss, utilize otherwise sensitive <strong>in</strong>gredients, <strong>in</strong>corporate unusual or<br />
time-release mechanisms <strong>in</strong>to the formulation, mask or preserve flavors and aromas,<br />
and transform liquids <strong>in</strong>to easily handled solid <strong>in</strong>gredients. Various techniques<br />
are employed to form microcapsules, <strong>in</strong>clud<strong>in</strong>g spray dry<strong>in</strong>g, spray chill<strong>in</strong>g<br />
or spray cool<strong>in</strong>g, extrusion coat<strong>in</strong>g, fluidized-bed coat<strong>in</strong>g, liposome entrapment,<br />
coacervation, <strong>in</strong>clusion complexation, centrifugal extrusion, and rotational<br />
suspension separation. <strong>Recent</strong> developments <strong>in</strong> each <strong>of</strong> these techniques are<br />
discussed <strong>in</strong> this review. Controlled release <strong>of</strong> food <strong>in</strong>gredients at the right place<br />
and the right time is a key functionality that can be provided by microencapsulation.<br />
A timely and targeted release improves the effectiveness <strong>of</strong> food additives, broadens<br />
the application range <strong>of</strong> food <strong>in</strong>gredients, and ensures optimal dosage, thereby<br />
improv<strong>in</strong>g the cost effectiveness for the food manufacturer. Reactive, sensitive, or<br />
volatile additives (vitam<strong>in</strong>s, cultures, flavors, etc.) can be turned <strong>in</strong>to stable <strong>in</strong>gredients<br />
through microencapsulation. With carefully f<strong>in</strong>e-tuned controlled-release<br />
properties, microencapsulation is no longer just an added-value technique, but the<br />
source <strong>of</strong> totally new <strong>in</strong>gredients with matchless properties.<br />
Keywords: <strong>Microencapsulation</strong>; <strong>Food</strong> <strong>in</strong>gredients; Controlled release; Spray<br />
dry<strong>in</strong>g; Microcapsules<br />
INTRODUCTION<br />
<strong>Microencapsulation</strong> is def<strong>in</strong>ed as a technology <strong>of</strong> packag<strong>in</strong>g solids,<br />
liquids, or gaseous materials <strong>in</strong> m<strong>in</strong>iature, sealed capsules that can release<br />
Correspondence: Hyun J<strong>in</strong> Park, Graduate School <strong>of</strong> Biotechnology, Korea<br />
University, 1, 5-Ka, Anam-Dong, Sungbuk-ku, Seoul 136–701, South Korea;<br />
Tel.: 82-2-3290-3450; Fax: 82-2-953-5892; E-mail: hjpark@korea.ac.kr
1362 Desai and Park<br />
their contents at controlled rates under specific conditions. [1–6] The<br />
microencapsulation technology has been used by the food <strong>in</strong>dustry for<br />
more than 60 years. In a broad sense, encapsulation technology <strong>in</strong> food<br />
process<strong>in</strong>g <strong>in</strong>cludes the coat<strong>in</strong>g <strong>of</strong> m<strong>in</strong>ute particles <strong>of</strong> <strong>in</strong>gredients (e.g.,<br />
acidulants, fats, and flavors) as well as whole <strong>in</strong>gredients (e.g., rais<strong>in</strong>s,<br />
nuts, and confectionary products), which may be accomplished by microencapsulation<br />
and macro-coat<strong>in</strong>g techniques, respectively. [7] More<br />
specifically, the microcapsule has the ability to preserve a substance <strong>in</strong><br />
the f<strong>in</strong>ely divided state and to release it as occasion demands. [8] These<br />
microcapsules may range from submicrometer to several millimeters <strong>in</strong><br />
size and have a multitude <strong>of</strong> different shapes, depend<strong>in</strong>g on the materials<br />
and methods used to prepare them. The food <strong>in</strong>dustry applies microencapsulation<br />
process for a variety <strong>of</strong> reasons: (1) encapsulation=<br />
entrapment can protect the core material from degradation by reduc<strong>in</strong>g<br />
its reactivity to its outside environment (e.g., heat, moisture, air, and<br />
light), (2) evaporation or transfer rate <strong>of</strong> the core material to the outside<br />
environment is decreased=retarded, (3) the physical characteristics <strong>of</strong> the<br />
orig<strong>in</strong>al material can be modified and made easier to handle, (4) the product<br />
can be tailor to either release slowly over time or at a certa<strong>in</strong> po<strong>in</strong>t<br />
(i.e., to control the release <strong>of</strong> the core material to achieve the property<br />
delay until the right stimulus), (5) the flavor <strong>of</strong> the core material can<br />
be masked, (6) the core material can be diluted when only very small<br />
amounts are required, yet still achieve a uniform dispersion <strong>in</strong> the host<br />
material, and (7) it can be employed to separate components with<strong>in</strong> a<br />
mixture that would otherwise react with one another. [9–14]<br />
Various properties <strong>of</strong> microcapsules that may be changed to suit specific<br />
<strong>in</strong>gredient applications <strong>in</strong>clude composition, mechanism <strong>of</strong> release,<br />
particle size, f<strong>in</strong>al physical form, and cost. The architecture <strong>of</strong> microcapsules<br />
is generally divided <strong>in</strong>to several arbitrary and overlapp<strong>in</strong>g classifications<br />
(Fig. 1). One such classification is known matrix encapsulation.<br />
This is the simplest structure, <strong>in</strong> which a sphere is surrounded by a wall<br />
or membrane <strong>of</strong> uniform thickness resembl<strong>in</strong>g that <strong>of</strong> a hen’s egg. In this<br />
design, the core material is buried to vary<strong>in</strong>g depths <strong>in</strong>side the shell. This<br />
microcapsule has been termed a s<strong>in</strong>gle-particle structure (Fig. 1A). It is<br />
also possible to design microcapsules that have several dist<strong>in</strong>ct cores<br />
with<strong>in</strong> the same microcapsule or, more commonly, number numerous<br />
core particles embedded <strong>in</strong> a cont<strong>in</strong>uous matrix <strong>of</strong> wall material. This<br />
type <strong>of</strong> design is termed the aggregate structure (Fig. 1B).<br />
In order to improve the properties <strong>of</strong> food <strong>in</strong>gredients, immobilization<br />
<strong>of</strong> food <strong>in</strong>gredients onto a suitable polymer or addition <strong>of</strong> antimicrobial<br />
agents are common practices <strong>in</strong> the food <strong>in</strong>dustres. [15–17] For<br />
example, an important bacteria used <strong>in</strong> the food <strong>in</strong>dustry, lactic acid bacteria,<br />
was first immobilized <strong>in</strong> 1975 on Berl saddles and Lactobacillus<br />
lactis was encapsulated <strong>in</strong> alg<strong>in</strong>ate gel beads years later. [18] Seiss and<br />
Davis suggested that immobilized lactic acid bacteria could be used to
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1363<br />
Figure 1. Schematic diagram <strong>of</strong> two representative types <strong>of</strong> microcapsules.<br />
cont<strong>in</strong>uously produce yogurt. [19] However, the alg<strong>in</strong>ate gel beads leaked<br />
large quantities <strong>of</strong> cells.<br />
The use <strong>of</strong> microencapsulated food <strong>in</strong>gredients allows food <strong>in</strong>gredients<br />
to be carefully tailored to the specific release site through the choice<br />
and microencapsulation variables, specifically, the method and food<br />
<strong>in</strong>gredients-polymer ratio. [7] The total amount <strong>of</strong> <strong>in</strong>gestion and the<br />
k<strong>in</strong>etics <strong>of</strong> release are variables that can be manipulated to achieve the<br />
desired result. [7,9,14] Us<strong>in</strong>g <strong>in</strong>novative microencapsulation technologies,<br />
and vary<strong>in</strong>g the copolymer ratio, molecular weight <strong>of</strong> the polymer, etc.,<br />
microcapsules can be developed <strong>in</strong>to an optimal food <strong>in</strong>gredient device. [7]<br />
Microcapsule-based systems <strong>in</strong>creases the life span <strong>of</strong> food <strong>in</strong>gredients<br />
and control the release <strong>of</strong> food <strong>in</strong>gredients.<br />
Various properties <strong>of</strong> microcapsules that may be changed to suit<br />
specific <strong>in</strong>gredient applications <strong>in</strong>clude composition, mechanism <strong>of</strong><br />
release, particle size, f<strong>in</strong>al physical form, and cost. Before consider<strong>in</strong>g<br />
the properties desired <strong>in</strong> encapsulated products, the purpose <strong>of</strong> encapsulation<br />
must be clear. In design<strong>in</strong>g the encapsulation process, the follow<strong>in</strong>g<br />
questions are taken <strong>in</strong>to consideration:<br />
1. What functionality should the encapsulated <strong>in</strong>gredients provide the<br />
f<strong>in</strong>al product?<br />
2. What k<strong>in</strong>d <strong>of</strong> coat<strong>in</strong>g material should be selected?<br />
3. What process<strong>in</strong>g conditions must the encapsulated <strong>in</strong>gredient survive<br />
before releas<strong>in</strong>g its content?<br />
4. What is optimal concentration <strong>of</strong> the active <strong>in</strong>gredient <strong>in</strong> the<br />
microcapsule?<br />
5. By what mechanism the <strong>in</strong>gredient be released from the<br />
microcapsules?<br />
6. What are the particle size, density, and stability requirements for the<br />
encapsulated <strong>in</strong>gredient?<br />
7. What are the cost constra<strong>in</strong>ts <strong>of</strong> the encapsulated <strong>in</strong>gredient?
1364 Desai and Park<br />
Controlled release may be def<strong>in</strong>ed as a method by which one or more<br />
active agents or <strong>in</strong>gredients are made available at a desired site and time<br />
at a specific rate. With the emergence <strong>of</strong> controlled-release technology, some<br />
heat-, temperature-, or pH-sensitive additives can be used very conveniently<br />
<strong>in</strong> food systems. Such additives are <strong>in</strong>troduced <strong>in</strong>to the food system mostly<br />
<strong>in</strong> the form <strong>of</strong> microcapsules. The additive present <strong>in</strong> the microcapsule is<br />
released under the <strong>in</strong>fluence <strong>of</strong> a specific stimulus at a specified stage. For<br />
example, flavors and nutrients may be released upon consumption, whereas<br />
sweeteners that are susceptible to heat may be released toward the end <strong>of</strong><br />
bak<strong>in</strong>g, thus prevent<strong>in</strong>g undesirable caramelization <strong>in</strong> the baked product.<br />
[20–30] Although quite a number <strong>of</strong> reviews are published on the microencapsulation<strong>of</strong>food<strong>in</strong>gredients,wehavemadeanattemptheretoupdate<br />
the recent developments <strong>in</strong> the microencapsulation <strong>of</strong> food <strong>in</strong>gredients.<br />
MICROENCAPSULATION TECHNIQUES<br />
Encapsulation <strong>of</strong> food <strong>in</strong>gredients <strong>in</strong>to coat<strong>in</strong>g materials can be achieved<br />
by several methods. The selection <strong>of</strong> the microencapsulation process is<br />
governed by the properties (physical and chemical) <strong>of</strong> core and coat<strong>in</strong>g<br />
materials and the <strong>in</strong>tended application <strong>of</strong> food <strong>in</strong>gredients. However,<br />
the microencapsulation processes that are used to encapsulate food <strong>in</strong>gredients<br />
are given <strong>in</strong> Table 1, which outl<strong>in</strong>es various methods used for the<br />
preparation <strong>of</strong> microencapsulated food systems. Sophisticated shell materials<br />
and technologies have been developed and an extremely wide variety<br />
<strong>of</strong> functionalities can now be achieved through microencapsulation. Any<br />
k<strong>in</strong>d <strong>of</strong> trigger can be used to prompt the release <strong>of</strong> the encapsulated<br />
<strong>in</strong>gredient, such as pH change (enteric and anti-enteric coat<strong>in</strong>g), mechanical<br />
stress, temperature, enzymatic activity, time, osmotic force, etc. However,<br />
cost considerations <strong>in</strong> the food <strong>in</strong>dustry are much more str<strong>in</strong>gent<br />
than <strong>in</strong>, for <strong>in</strong>stance, the pharmaceutical or cosmetic <strong>in</strong>dustries. The<br />
selection <strong>of</strong> microencapsulation method and coat<strong>in</strong>g materials are <strong>in</strong>terdependent.<br />
Based on the coat<strong>in</strong>g material or method applied, the appropriate<br />
method or coat<strong>in</strong>g material is selected. Coat<strong>in</strong>g materials, which<br />
are basically film-form<strong>in</strong>g materials, can be selected from a wide variety<br />
<strong>of</strong> natural or synthetic polymers, depend<strong>in</strong>g on the material to be coated<br />
and characteristics desired <strong>in</strong> the f<strong>in</strong>al microcapsules.<br />
The composition <strong>of</strong> the coat<strong>in</strong>g material is the ma<strong>in</strong> determ<strong>in</strong>ant <strong>of</strong><br />
the functional properties <strong>of</strong> the microcapsule and <strong>of</strong> how it may be used<br />
to improve the performance <strong>of</strong> a particular <strong>in</strong>gredient. An ideal coat<strong>in</strong>g<br />
material should exhibit the follow<strong>in</strong>g characteristics:<br />
1. Good rheological properties at high concentration and easy workability<br />
dur<strong>in</strong>g encapsulation.<br />
2. The ability to disperse or emulsify the active material and stabilize the<br />
emulsion produced.
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1365<br />
Table 1. Various microencapsulation techniques and the processes <strong>in</strong>volved <strong>in</strong><br />
each technique<br />
No <strong>Microencapsulation</strong> technique Major steps <strong>in</strong> encapsulation<br />
1 Spray-dry<strong>in</strong>g a. Preparation <strong>of</strong> the dispersion<br />
b. Homogenization <strong>of</strong> the dispersion<br />
c. Atomization <strong>of</strong> the <strong>in</strong>feed dispersion<br />
d. Dehydration <strong>of</strong> the atomized particles<br />
2 Spray-cool<strong>in</strong>g a. Preparation <strong>of</strong> the dispersion<br />
b. Homogenization <strong>of</strong> the dispersion<br />
c. Atomization <strong>of</strong> the <strong>in</strong>feed dispersion<br />
3 Spray-chill<strong>in</strong>g a. Preparation <strong>of</strong> the dispersion<br />
b. Homogenization <strong>of</strong> the dispersion<br />
c. Atomization <strong>of</strong> the <strong>in</strong>feed dispersion<br />
4 Fluidized-bed coat<strong>in</strong>g a. Preparation <strong>of</strong> coat<strong>in</strong>g solution<br />
b. Fluidization <strong>of</strong> core particles.<br />
c. Coat<strong>in</strong>g <strong>of</strong> core particles<br />
5 Extrusion a. Preparation <strong>of</strong> molten coat<strong>in</strong>g solution<br />
b. Dispersion <strong>of</strong> core <strong>in</strong>to molten<br />
polymer<br />
c. Cool<strong>in</strong>g or pass<strong>in</strong>g <strong>of</strong> core-coat<br />
mixture through dehydrat<strong>in</strong>g liquid<br />
6 Centrifugal extrusion a. Preparation <strong>of</strong> core solution<br />
b. Preparation <strong>of</strong> coat<strong>in</strong>g material<br />
solution<br />
c. Co-extrusion <strong>of</strong> core and coat<br />
solution through nozzles<br />
7 Lyophilization a. Mix<strong>in</strong>g <strong>of</strong> core <strong>in</strong> a coat<strong>in</strong>g solution<br />
b. Freeze-dry<strong>in</strong>g <strong>of</strong> the mixture<br />
8 Coacervation a. Formation <strong>of</strong> a three-immiscible<br />
chemical phases<br />
b. Deposition <strong>of</strong> the coat<strong>in</strong>g<br />
9 Centrifugal suspension<br />
separation<br />
c. Solidification <strong>of</strong> the coat<strong>in</strong>g<br />
a. Mix<strong>in</strong>g <strong>of</strong> core <strong>in</strong> a coat<strong>in</strong>g material<br />
b. Pour the mixture over a rotat<strong>in</strong>g disc<br />
to obta<strong>in</strong> encapsulated t<strong>in</strong>y particles<br />
c. Dry<strong>in</strong>g<br />
10 Cocrystallization a. Preparation <strong>of</strong> supersaturated<br />
sucrose solution<br />
b. Add<strong>in</strong>g <strong>of</strong> core <strong>in</strong>to supersaturated<br />
solution<br />
c. Emission <strong>of</strong> substantial heat after<br />
solution reaches the sucrose<br />
crystallization temperature<br />
(Cont<strong>in</strong>ued)
1366 Desai and Park<br />
Table 1. (Cont<strong>in</strong>ued)<br />
No <strong>Microencapsulation</strong> technique Major steps <strong>in</strong> encapsulation<br />
11 Liposome entrapment a. Micr<strong>of</strong>luidization<br />
b. Ultrasonication<br />
c. Reverse-phase evaporation<br />
12 Inclusion complexation Preparation <strong>of</strong> complexes by mix<strong>in</strong>g or<br />
gr<strong>in</strong>d<strong>in</strong>g or spray-dry<strong>in</strong>g<br />
3. Nonreactivity with the material to be encapsulated both dur<strong>in</strong>g process<strong>in</strong>g<br />
and on prolonged storage.<br />
4. The ability to seal and hold the active material with<strong>in</strong> its structure<br />
dur<strong>in</strong>g process<strong>in</strong>g or storage.<br />
5. The ability to completely release the solvent or other materials used<br />
dur<strong>in</strong>g the process <strong>of</strong> encapsulation under dry<strong>in</strong>g or other desolventization<br />
conditions.<br />
6. The ability to provide maximum protection to the active material<br />
aga<strong>in</strong>st environmental conditions (e.g., oxygen, heat, light, humidity).<br />
7. Solubility <strong>in</strong> solvents acceptable <strong>in</strong> the food <strong>in</strong>dustry (e.g., water,<br />
ethanol).<br />
8. Chemical nonreactivity with the active core materials.<br />
9. Inexpensive, food-grade status.<br />
Because no s<strong>in</strong>gle coat<strong>in</strong>g material can meet all <strong>of</strong> the criteria listed<br />
above, <strong>in</strong> practice either coat<strong>in</strong>g materials are employed <strong>in</strong> comb<strong>in</strong>ations<br />
or modifiers such as oxygen scavengers, antioxidants, chelat<strong>in</strong>g agents,<br />
and surfactants are added. Some commonly used biocompatible and<br />
food-grade coat<strong>in</strong>g materials are listed <strong>in</strong> Table 2. However, chemical<br />
modifications <strong>of</strong> the exist<strong>in</strong>g coat<strong>in</strong>g materials to manipulate their<br />
properties are also be<strong>in</strong>g considered. Those modified coat<strong>in</strong>g materials<br />
exhibit better physical and mechanical properties when compared to <strong>in</strong>dividual<br />
coat<strong>in</strong>g materials.<br />
Spray-Dry<strong>in</strong>g<br />
Spray-dry<strong>in</strong>g encapsulation has been used <strong>in</strong> the food <strong>in</strong>dustry s<strong>in</strong>ce the<br />
late 1950s to provide flavor oils with some protection aga<strong>in</strong>st degradation=oxidation<br />
and to convert liquids to powders. Spray-dry<strong>in</strong>g is the<br />
most widely used microencapsulation technique <strong>in</strong> the food <strong>in</strong>dustry<br />
and is typically used for the preparation <strong>of</strong> dry, stable food additives<br />
and flavors. The process is economical; flexible, <strong>in</strong> that it <strong>of</strong>fers substantial<br />
variation <strong>in</strong> microencapsulation matrix; adaptable to commonly used<br />
process<strong>in</strong>g equipment; and produces particles <strong>of</strong> good quality. In fact,
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1367<br />
Table 2. Coat<strong>in</strong>g materials for microencapsulation <strong>of</strong> functional food additives<br />
Category Coat<strong>in</strong>g materials<br />
Carbohydrate Starch,maltodextr<strong>in</strong>s,<br />
chitosan,<br />
corn syrup solids,<br />
dextran, modified<br />
starch, cyclodextr<strong>in</strong>s<br />
Cellulose Carboxymethylcellulose,<br />
methyl cellulose,<br />
ethylcellulose,<br />
celluloseacetate-phthalate,<br />
celluloseacetatebutylate-phthalate<br />
Gum Gum acacia, agar, sodium<br />
alg<strong>in</strong>ate, carrageenan<br />
Lipids Wax, paraff<strong>in</strong>, beeswax,<br />
diacylglyerols, oils, fats<br />
Prote<strong>in</strong> Gluten, case<strong>in</strong>, gelat<strong>in</strong>,<br />
album<strong>in</strong>, peptides<br />
Widely used<br />
methods References<br />
Spray- and<br />
freeze-dry<strong>in</strong>g,<br />
extrusion,<br />
coacervation,<br />
<strong>in</strong>clusion<br />
complexation<br />
Coacervation,<br />
spray-dry<strong>in</strong>g,<br />
and edible films<br />
20–24<br />
25–26<br />
Spray-dry<strong>in</strong>g, syr<strong>in</strong>ge 27<br />
method (gel beads)<br />
Emulsion, liposomes, 28–29<br />
film formation<br />
Emulsion, spray-dry<strong>in</strong>g 30<br />
spray-dry<strong>in</strong>g production costs are lower than those associated with most<br />
other methods <strong>of</strong> encapsulation. One limitation <strong>of</strong> the spray-dry<strong>in</strong>g technology<br />
is the limited number <strong>of</strong> shell materials available. S<strong>in</strong>ce almost all<br />
spray-dry<strong>in</strong>g processes <strong>in</strong> the food <strong>in</strong>dustry are carried out from aqueous<br />
feed formulations, the shell material must be soluble <strong>in</strong> water at an<br />
acceptable level. Typical shell materials <strong>in</strong>clude gum acacia, maltodextr<strong>in</strong>s,<br />
hydrophobically modified starch, and mixtures there<strong>of</strong>. Other polysaccharides<br />
(alg<strong>in</strong>ate, carboxymethylcellulose, guar gum) and prote<strong>in</strong>s<br />
(whey prote<strong>in</strong>s, soy prote<strong>in</strong>s, sodium case<strong>in</strong>ate) can be used as the wall<br />
material <strong>in</strong> spray-dry<strong>in</strong>g, but their usage becomes very tedious and<br />
expensive because <strong>of</strong> their low solubility <strong>in</strong> water: the amount <strong>of</strong> water<br />
<strong>in</strong> the feed to be evaporated is much larger due to the lower dry matter<br />
content and the amount <strong>of</strong> active <strong>in</strong>gredient <strong>in</strong> the feed must be reduced<br />
accord<strong>in</strong>gly. In this method, the material for encapsulation is homogenized<br />
with the carrier material at a different ratio. The mixture is then<br />
fed <strong>in</strong>to a spray dryer and atomized with a nozzle or sp<strong>in</strong>n<strong>in</strong>g wheel.<br />
Water is evaporated by the hot air contact<strong>in</strong>g the atomized material.<br />
The microcapsules are then collected after they fall to the bottom <strong>of</strong><br />
the drier. [31]<br />
Rosenberg and Sheu demonstrated the use <strong>of</strong> whey prote<strong>in</strong> isolate as<br />
a wall material for encapsulation <strong>of</strong> volatiles. [32] They encapsulated ethyl<br />
butyrate and ethyl caprylate <strong>in</strong> whey prote<strong>in</strong> isolate and 1:1 mixture <strong>of</strong>
1368 Desai and Park<br />
whey prote<strong>in</strong> isolate and lactose. Retention <strong>of</strong> volatiles was significantly<br />
affected by wall solids concentration (10–30%, w=w), <strong>in</strong>itial ester load<br />
(10–75%,w=w, <strong>of</strong> wall solids), and by ester and wall type. Ester retention<br />
<strong>in</strong> whey prote<strong>in</strong> isolate=lactose was higher than <strong>in</strong> whey prote<strong>in</strong> isolate.<br />
Spray-dry<strong>in</strong>g is a food manufacturer–friendly technique because it allows<br />
the food processor to manipulate the preparation process to improve the<br />
quality <strong>of</strong> the f<strong>in</strong>al product. <strong>Recent</strong>ly, Shiga et al. prepared flavor<strong>in</strong>clusion<br />
powder by a spray-dry<strong>in</strong>g technique us<strong>in</strong>g the comb<strong>in</strong>ed encapsulation<br />
method <strong>of</strong> <strong>in</strong>clusion by b-cyclodextr<strong>in</strong> and emulsified by gum<br />
arabic where d-limonene and ethyl n-hexanoate were used as model<br />
flavors. [33] The effective film-form<strong>in</strong>g property and <strong>in</strong>clusion complex<br />
were achieved by apply<strong>in</strong>g high pressure to the mixture <strong>of</strong> flavors and<br />
b-cyclodextr<strong>in</strong> slurry us<strong>in</strong>g a micr<strong>of</strong>luidizer. It is reported that flavor<br />
retention dur<strong>in</strong>g spray-dry<strong>in</strong>g <strong>in</strong>creased due to blend<strong>in</strong>g <strong>of</strong> gum arabic<br />
and b-cyclodextr<strong>in</strong> <strong>in</strong> the feed liquid. The release rate <strong>of</strong> flavors was<br />
manipulated by the blend<strong>in</strong>g <strong>of</strong> maltodextr<strong>in</strong> <strong>in</strong> the feed liquid. In order<br />
to evaluate the release k<strong>in</strong>etics <strong>of</strong> flavors, the release data were fitted to<br />
Avrami’s equation (Eq. 1).<br />
R ¼ exp½ ðktÞ n Š ð1Þ<br />
where R is the retention <strong>of</strong> flavors dur<strong>in</strong>g release, t is time, n is a parameter<br />
represent<strong>in</strong>g the release mechanism, and k is the release rate constant.<br />
Eq. (1) was orig<strong>in</strong>ally developed the crystal growth <strong>of</strong> polymers,<br />
and has been recently used to represent the time-dependent prote<strong>in</strong><br />
<strong>in</strong>activation <strong>in</strong> amorphous sugar matrices. [34] In Eq. (1), n ¼ 1 represents<br />
the first-order reaction, and n ¼ 0.54 represents the diffusion-limit<strong>in</strong>g<br />
reaction k<strong>in</strong>etics. [35] Tak<strong>in</strong>g a logarithm <strong>of</strong> both sides <strong>of</strong> Eq. (1) twice<br />
yields Eq. (2):<br />
lnð ln RÞ ¼n ln k þ n ln t ð2Þ<br />
From Eq. (2) one can f<strong>in</strong>d the parameter n as a slope by plott<strong>in</strong>g ln( ln<br />
R) vs.lnt, and the release rate constant k from the <strong>in</strong>terception at ln t ¼ 0.<br />
It is important to protect the flavor loss dur<strong>in</strong>g dry<strong>in</strong>g, because<br />
high-temperature air is commonly used <strong>in</strong> spray-dry<strong>in</strong>g. Generally, the<br />
retention <strong>of</strong> flavor <strong>in</strong> microcapsules is manipulated by vary<strong>in</strong>g the<br />
spray-dry<strong>in</strong>g conditions and compositions <strong>of</strong> wall material. <strong>Recent</strong>ly,<br />
Liu et al. adopted new technique where they used emulsified liquid flavor<br />
for spray-dry<strong>in</strong>g. [36] Nearly 100% <strong>of</strong> d-limonene was reta<strong>in</strong>ed dur<strong>in</strong>g<br />
spray-dry<strong>in</strong>g, <strong>in</strong>dependent <strong>of</strong> the composition <strong>of</strong> the feed liquid. However,<br />
the stability <strong>of</strong> emulsion droplets markedly affected the retention<br />
<strong>of</strong> flavors. d-Limonene emulsion was quite stable <strong>in</strong>dependent <strong>of</strong> the<br />
emulsifier, while the emulsion <strong>of</strong> ethyl butyrate was unstable with gum<br />
arabic as the emulsifier. The use <strong>of</strong> a mixture <strong>of</strong> gum arabic and soluble<br />
soybean polysaccharide as the emulsifier improved oil<strong>in</strong>ess, and adjust<strong>in</strong>g
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1369<br />
density <strong>of</strong> ethyl butyrate and add<strong>in</strong>g gelat<strong>in</strong> <strong>in</strong>creased the retention <strong>of</strong><br />
ethyl butyrate dur<strong>in</strong>g spray-dry<strong>in</strong>g.<br />
In recent years, new wall materials for use <strong>in</strong> spray-dry<strong>in</strong>g microencapsulation<br />
have not really emerged. A few exceptions are noteworthy,<br />
though. The <strong>in</strong>vestigations <strong>of</strong> other natural gums and their emulsification<br />
and shell properties have been reported. Mesquite gum, for <strong>in</strong>stance, has<br />
been shown to give a better stability <strong>of</strong> the o=w emulsions and higher<br />
encapsulation efficiency compared to gum acacia. [37,38] August<strong>in</strong> et al.<br />
proposed the use <strong>of</strong> Maillard reaction products (MRPs) obta<strong>in</strong>ed by<br />
the reaction at high temperature between prote<strong>in</strong> and carbohydrate to<br />
encapsulate oxidation-sensitive nutrients such as fish oils. [39] The MRPs<br />
are known to exhibit antioxidant properties and form a stable and robust<br />
shell around the oil phase. The stability <strong>of</strong> the oil aga<strong>in</strong>st oxidation was<br />
greatly improved compared to nonencapsulated spray-dried samples <strong>in</strong><br />
ord<strong>in</strong>ary shell material. More <strong>in</strong>terest<strong>in</strong>g is the recent development <strong>of</strong><br />
complex shell formulations for spray-dry<strong>in</strong>g encapsulation. For <strong>in</strong>stance,<br />
aqueous two-phase systems (ATPSs), which result from the phase separation<br />
<strong>of</strong> a mixture <strong>of</strong> soluble polymers <strong>in</strong> a common solvent due to the<br />
low entropy <strong>of</strong> mix<strong>in</strong>g (DS mix) <strong>of</strong> polymer mixtures, can be used to design<br />
double-encapsulated <strong>in</strong>gredients <strong>in</strong> a s<strong>in</strong>gle spray-dry<strong>in</strong>g step. Millqvist-<br />
Fureby et al. encapsulated Enterococcus fæcium <strong>in</strong> a mixture <strong>of</strong> polyv<strong>in</strong>ylpyrrolidone<br />
(PVP) and dextran. [40] While prote<strong>in</strong>s exhibit partition<strong>in</strong>g<br />
between the two phases, whole cells tend to concentrate <strong>in</strong> one <strong>of</strong> the<br />
polymer phases, which make them ideal candidates for ATPS spray-dry<strong>in</strong>g.<br />
The structure <strong>of</strong> the microcapsule, whether PVP is the outer layer and<br />
dextran the <strong>in</strong>ner core or vice versa, can be controlled by adjust<strong>in</strong>g the ratio<br />
and concentration <strong>of</strong> the two polymers. Encapsulated E. fæcium <strong>in</strong> spraydried<br />
ATPS showed a survival rate <strong>of</strong> up to 45% after4weeksatroom<br />
temperature. Another example is the preparation and spray-dry<strong>in</strong>g <strong>of</strong> multiple<br />
emulsions, which results a <strong>in</strong> a double-layered microcapsule, provid<strong>in</strong>g<br />
better protection to sensitive materials such as oxidation-probe flavor oils.<br />
Edris and Bergmtahl have encapsulated orange oil by first prepar<strong>in</strong>g a triple<br />
emulsion o=w=o=w and then evaporat<strong>in</strong>g the outer cont<strong>in</strong>uous aqueous<br />
phase, which conta<strong>in</strong>s sodium case<strong>in</strong>ate and lactose as shell material, by<br />
spray-dry<strong>in</strong>g. [41] The process leads to a dry free-flow<strong>in</strong>g powder constitut<strong>in</strong>g<br />
<strong>of</strong> a double o=w=o, <strong>in</strong> which the <strong>in</strong>ner orange oil phase is dispersed <strong>in</strong> an<br />
aqueous phase, which is itself dispersed <strong>in</strong> an oil phase encapsulated <strong>in</strong><br />
sodium case<strong>in</strong>ate and lactose. This double emulsion process is not practically<br />
more complex than a typical spray-dry<strong>in</strong>g process that requires an<br />
emulsion step anyway. However, prepar<strong>in</strong>g a second emulsion implies a<br />
dilution <strong>of</strong> the flavor oil, and the much lower payload <strong>in</strong> the microcapsule<br />
(5–10%) is a drawback compared to typical spray-dried flavor oils, which<br />
have payloads <strong>of</strong> around 20–25%. The unique protection and delayedrelease<br />
properties obta<strong>in</strong>ed with two layers might compensate for the lower<br />
payload, but this has still to be demonstrated.
1370 Desai and Park<br />
Chitosan is a hydrophilic, biocompatible, and biodegradable, polysaccharide<br />
<strong>of</strong> low toxicity. In recent years, it has been used for development<br />
<strong>of</strong> oral controlled drug delivery systems. It is also a well-known<br />
dietary food additive. Therefore, our research team demonstrated the<br />
cross-l<strong>in</strong>ked chitosan as a wall material for the encapsulation <strong>of</strong> vitam<strong>in</strong><br />
C by a spray-dry<strong>in</strong>g technique. Vitam<strong>in</strong> C, a representative water-soluble<br />
vitam<strong>in</strong>, has a variety <strong>of</strong> biological, pharmaceutical, and dermatological<br />
functions. Vitam<strong>in</strong> C is widely used <strong>in</strong> various types <strong>of</strong> foods as a vitam<strong>in</strong><br />
supplement and as an antioxidant. Hence, <strong>in</strong> previous studies, susta<strong>in</strong>edrelease<br />
carriers <strong>of</strong> vitam<strong>in</strong> C have been prepared by us<strong>in</strong>g cross-l<strong>in</strong>ked<br />
chitosan as a wall material by spray-dry<strong>in</strong>g technique. [42–44] The process<br />
<strong>of</strong> the preparation <strong>of</strong> vitam<strong>in</strong> C–encapsulated chitosan microcapsules is<br />
shown <strong>in</strong> Fig. 2. Chitosan was cross-l<strong>in</strong>ked with nontoxic cross-l<strong>in</strong>k<strong>in</strong>g<br />
agent, i.e., tripolyphosphate. Vitam<strong>in</strong> C–encapsulated chitosan microspheres<br />
<strong>of</strong> different size, surface morphology, load<strong>in</strong>g efficiency, and zeta<br />
potential with controlled-release property could be obta<strong>in</strong>ed by vary<strong>in</strong>g<br />
the manufactur<strong>in</strong>g parameters (<strong>in</strong>let temperature, flow rate) and us<strong>in</strong>g<br />
the different molecular weight and concentration <strong>of</strong> chitosan. Vitam<strong>in</strong><br />
C–encapsulated chitosan microcapsules were spherical <strong>in</strong> shape with a<br />
smooth surface as observed by scann<strong>in</strong>g electron microscopy (Fig. 3).<br />
<strong>Microencapsulation</strong> <strong>of</strong> vitam<strong>in</strong> C improves and broadens its applications<br />
<strong>in</strong> the food <strong>in</strong>dustry.<br />
Figure 2. Procedure <strong>of</strong> preparation <strong>of</strong> vitam<strong>in</strong> C–encapsulated chitosan<br />
microspheres by spray-dry<strong>in</strong>g.
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1371<br />
Figure 3. Scann<strong>in</strong>g electronic microscopic picture <strong>of</strong> the vitam<strong>in</strong> C-encapsulated<br />
microcapsule.<br />
Numerous materials have been used as flavor-encapsulat<strong>in</strong>g agents<br />
us<strong>in</strong>g a spray-dry<strong>in</strong>g technique. These <strong>in</strong>clude prote<strong>in</strong>s, gums, and modified<br />
starches. [45] An area <strong>of</strong> research <strong>of</strong> <strong>in</strong>creas<strong>in</strong>g <strong>in</strong>terest is the development<br />
<strong>of</strong> alternative and <strong>in</strong>expensive polymers that may be considered<br />
natural, like gum arabic, and that could encapsulate flavors with the<br />
same efficiency as gum arabic. [46] Mesquite gum has been reported as a<br />
very good encapsulat<strong>in</strong>g agent. [47,48] Berista<strong>in</strong> and Vernon-Carter noted<br />
that a blend <strong>of</strong> 60% gum arabic and 40% mesquite gum encapsulated<br />
93.5% <strong>of</strong> orange peel oil. [49] More recently, Berista<strong>in</strong> et al. reported that<br />
a mixture consist<strong>in</strong>g <strong>of</strong> 40% mesquite gum and 60% maltodextr<strong>in</strong>s was<br />
able to encapsulate 84.6% <strong>of</strong> the start<strong>in</strong>g oil. [50] Cardamom-based oil<br />
microcapsules were successfully produced by spray-dry<strong>in</strong>g us<strong>in</strong>g mesquite<br />
gum. [38] The stability aga<strong>in</strong>st drop coalescence <strong>of</strong> the emulsions was elevated<br />
for all the gum:oil ratios studied. High flavor retention (83.6%) was<br />
atta<strong>in</strong>ed dur<strong>in</strong>g microencapsulation by spray-dry<strong>in</strong>g when a proportion<br />
<strong>of</strong> 4:1 gum:oil was used. This confirmed the <strong>in</strong>terest<strong>in</strong>g emulsify<strong>in</strong>g<br />
properties and good flavor-encapsulation ability that qualify mesquite<br />
gum as an important alternative encapsulat<strong>in</strong>g medium. The microcapsules<br />
can be readily used as a food <strong>in</strong>gredient.<br />
<strong>Recent</strong> developments have been <strong>in</strong> the use <strong>of</strong> new carrier materials<br />
and a newly designed spray dryer. Colloides Naturels and TIC Gums
1372 Desai and Park<br />
have developed new comb<strong>in</strong>ations <strong>of</strong> gum arabic starches to <strong>in</strong>crease<br />
the retention <strong>of</strong> volatiles and shelf life <strong>of</strong> microcapsules. [51,52] Risch and<br />
Re<strong>in</strong>eccius enhanced the retention <strong>of</strong> orange oil and decreased oxidation<br />
by us<strong>in</strong>g gum arabic. [53] Bhandari et al. showed that a new type <strong>of</strong> dryer<br />
called the Leaflish spray dryer, which uses a high air velocity with a temperature<br />
<strong>of</strong> 300 to 400 C, was effective for encapsulat<strong>in</strong>g citral and l<strong>in</strong>alyl<br />
acetate without degradation. [54] A disadvantage is that a separate<br />
agglomeration step is required to prevent separation or to render the<br />
obta<strong>in</strong>ed powder soluble. A chief advantage is that this technique can<br />
be used for heat-labile materials. <strong>Recent</strong>ly, studies on the modification<br />
<strong>of</strong> spray-dry<strong>in</strong>g chamber configurations and atomization along applications<br />
<strong>of</strong> computational fluid dynamic model have been reported to<br />
broaden the applications range <strong>of</strong> spray-dry<strong>in</strong>g methods. [55–60]<br />
Spray-Chill<strong>in</strong>g or Spray-Cool<strong>in</strong>g<br />
In spray-chill<strong>in</strong>g and spray-cool<strong>in</strong>g, the core and wall mixtures are<br />
atomized <strong>in</strong>to the cooled or chilled air, which causes the wall to solidify<br />
around the core. Unlike spray-dry<strong>in</strong>g, spray-chill<strong>in</strong>g or spray-cool<strong>in</strong>g<br />
does not <strong>in</strong>volve evaporation <strong>of</strong> water. In spray-cool<strong>in</strong>g, the coat<strong>in</strong>g<br />
material is typically some form <strong>of</strong> vegetable oil or its derivatives. However,<br />
a wide range <strong>of</strong> other encapsulat<strong>in</strong>g materials may be employed.<br />
These <strong>in</strong>clude fat and stear<strong>in</strong> with melt<strong>in</strong>g po<strong>in</strong>ts <strong>of</strong> 45–122 C, as well<br />
as hard mono- and diacylglycerols with melt<strong>in</strong>g po<strong>in</strong>ts <strong>of</strong> 45–65 C. [31]<br />
In spray-chill<strong>in</strong>g, the coat<strong>in</strong>g material is typically a fractionated or hydrogenated<br />
vegetable oil with a melt<strong>in</strong>g po<strong>in</strong>t <strong>in</strong> the range <strong>of</strong> 32–42 C. [61] In<br />
spray-chill<strong>in</strong>g, there is no mass transfer (i.e., evaporation from the atomized<br />
droplets); therefore these solidify <strong>in</strong>to almost perfect spheres to<br />
give free-flow<strong>in</strong>g powders. Atomization gives an enormous surface area<br />
and an immediate as well as <strong>in</strong>timate mix<strong>in</strong>g <strong>of</strong> these droplets with the<br />
cool<strong>in</strong>g medium. Microcapsules prepared by spray-chill<strong>in</strong>g and spraycool<strong>in</strong>g<br />
are <strong>in</strong>soluble <strong>in</strong> water due to the lipid coat<strong>in</strong>g. Consequently,<br />
these techniques tend to be utilized for encapsulat<strong>in</strong>g water-soluble core<br />
materials such as m<strong>in</strong>erals, water-soluble vitam<strong>in</strong>s, enzymes, acidulants,<br />
and some flavors. [62]<br />
Fluidized-Bed Coat<strong>in</strong>g<br />
Orig<strong>in</strong>ally developed as a pharmaceutical technique, fluidized-bed coat<strong>in</strong>g<br />
is now <strong>in</strong>creas<strong>in</strong>gly be<strong>in</strong>g applied <strong>in</strong> the food <strong>in</strong>dustry to f<strong>in</strong>e-tune<br />
the effect <strong>of</strong> functional <strong>in</strong>gredients and additives. The ma<strong>in</strong> benefits <strong>of</strong><br />
such m<strong>in</strong>iature packages, called microcapsules, <strong>in</strong>clude <strong>in</strong>creased shelf<br />
life, taste mask<strong>in</strong>g, ease <strong>of</strong> handl<strong>in</strong>g, controlled release, and improved<br />
aesthetics, taste, and color. Fluidized-bed coat<strong>in</strong>g <strong>in</strong>creas<strong>in</strong>gly supplies
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1373<br />
the food <strong>in</strong>dustry with a wide variety <strong>of</strong> encapsulated versions <strong>of</strong> food<br />
<strong>in</strong>gredients and additives. [63] Compared to pharmaceutical fluidized-bed<br />
coat<strong>in</strong>g, food <strong>in</strong>dustry fluidized-bed coat<strong>in</strong>g is more obliged to cut<br />
production costs and, therefore, should adopt a somewhat different<br />
approach to this rather expensive technology. Solid particles are suspended<br />
<strong>in</strong> a temperature and humidity-controlled chamber <strong>of</strong> highvelocity<br />
air where the coat<strong>in</strong>g material is atomized. [64,65] Typical food<br />
process<strong>in</strong>g applications <strong>of</strong> fluidization <strong>in</strong>clude freez<strong>in</strong>g and cool<strong>in</strong>g, dry<strong>in</strong>g,<br />
puff<strong>in</strong>g, freeze-dry<strong>in</strong>g, spray-dry<strong>in</strong>g, agglomeration and granulation,<br />
classification, and blanch<strong>in</strong>g and cook<strong>in</strong>g. [66] Great variations <strong>in</strong> available<br />
wall materials exist. Cellulose derivatives, dextr<strong>in</strong>s, emulsifiers,<br />
lipids, prote<strong>in</strong> derivatives, and starch derivatives are examples <strong>of</strong> typical<br />
coat<strong>in</strong>g systems, and they may be used <strong>in</strong> a molten state or dissolved <strong>in</strong> an<br />
evaporable solvent. This technique is applicable for hot-melt coat<strong>in</strong>gs<br />
such as hydrogenated vegetable oil, stear<strong>in</strong>es, fatty acids, emulsifiers,<br />
and waxes, or solvent-based coat<strong>in</strong>gs such as starches, gums, maltodextr<strong>in</strong>s.<br />
For hot melts, cool air is used to harden the carrier, whereas for<br />
solvent-based coat<strong>in</strong>gs, hot air is used to evaporate the solvent. Hot-melt<br />
<strong>in</strong>gredients release their contents by <strong>in</strong>creas<strong>in</strong>g the temperature or physical<br />
breakage, whereas water-soluble coat<strong>in</strong>gs release their contents when<br />
water is added. Fluidized-bed encapsulation can be used to isolate iron<br />
from ascorbic acid <strong>in</strong> multivitam<strong>in</strong>s and <strong>in</strong> small tablets such as children’s<br />
vitam<strong>in</strong>s. Many fortified foods, nutritional mixes, and dry mixes, conta<strong>in</strong><br />
fluidized-bed–encapsulated <strong>in</strong>gredients. Citric acid, lactic acid, sorbic<br />
acid, vitam<strong>in</strong> C, sodium bicarbonate <strong>in</strong> baked goods, and salt added to<br />
pretzels and meats are all encapsulated. Nowadays, the applicability<br />
and the utility <strong>of</strong> fluidized-bed coat<strong>in</strong>g and other microencapsulation<br />
techniques <strong>in</strong> the food <strong>in</strong>dustry is well recognized, as presented <strong>in</strong> several<br />
reviews. [66–70] There are, however, important factors to be considered <strong>in</strong><br />
fluidized-bed coat<strong>in</strong>g <strong>of</strong> food <strong>in</strong>gredients and additives.<br />
Fluidized-bed coat<strong>in</strong>g was first developed by D.E. Wurster <strong>in</strong> the<br />
1950s; hence, the term ‘‘Wurster process.’’ [70] Today, the fluidized-bed<br />
coat<strong>in</strong>g method is be<strong>in</strong>g modified by chang<strong>in</strong>g the position <strong>of</strong> the nozzle<br />
to be used for coat<strong>in</strong>g the solid particles. The different fluidized-bed coat<strong>in</strong>g<br />
methods are: (1) top-spray, (2) bottom-spray, and (3) tangentialspray.<br />
The conventional top-spray method is shown <strong>in</strong> Fig. 4. The air<br />
is passed through a bed <strong>of</strong> core particles to suspend them <strong>in</strong> air and coat<strong>in</strong>g<br />
solution is sprayed countercurrently onto the randomly fluidized<br />
particles. The coated particles travel through the coat<strong>in</strong>g zone <strong>in</strong>to the<br />
expansion chamber, and then they fall back <strong>in</strong>to the product conta<strong>in</strong>er<br />
and cont<strong>in</strong>ue cycl<strong>in</strong>g throughout the process. [71] The top-spray system<br />
has successfully been used to coat materials as small as 100 mm. [71] However,<br />
Thiel and Nguyen demonstrated the possibility <strong>of</strong> encapsulat<strong>in</strong>g<br />
very f<strong>in</strong>e particles (2–5 mm) by adsorb<strong>in</strong>g them on a coarser carrier, which<br />
is encapsulated by means <strong>of</strong> conventional fluidized-bed equipment. [72] In
1374 Desai and Park<br />
Figure 4. Top-spray fluidized-bed coat<strong>in</strong>g.<br />
the top-spray configuration, controll<strong>in</strong>g the distance the droplets travel<br />
before contact<strong>in</strong>g the substrate is impossible, and coat<strong>in</strong>g imperfections<br />
can occur due to premature droplet evaporation.<br />
The bottom-spray method known as the Wurster system (Fig. 5) is<br />
widely used for coat<strong>in</strong>g particles as small as 100 mm. In this method,<br />
the particles are recycled through the coat<strong>in</strong>g zone at a faster rate and<br />
the fluidization pattern is much more controlled than the top-spray<br />
method. [73] The typical advantage <strong>of</strong> this method is that, the path <strong>of</strong><br />
the droplets concurrently toward the core particles is extremely short,<br />
Figure 5. Bottom-spray fluidized-bed coat<strong>in</strong>g.
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1375<br />
so that premature droplet evaporation is almost absent. In addition,<br />
coat<strong>in</strong>g solution can spread out at the lowest viscosity, produc<strong>in</strong>g a very<br />
dense film with a superior physical strength. In contrary, Wesdyk et al.<br />
reported that particles coated <strong>in</strong> the bottom spray mode did not display<br />
a uniform film thickness with respect to particle size; larger beads displayed<br />
thicker films compared with smaller beads. The film thickness<br />
variation could be expla<strong>in</strong>ed by differences <strong>in</strong> fluidization patterns. This<br />
phenomenon did not occur <strong>in</strong> other configurations. [74]<br />
<strong>Recent</strong>ly, a fasc<strong>in</strong>at<strong>in</strong>g advancement <strong>in</strong> fluidized-bed coat<strong>in</strong>g technique<br />
was reported by Matsuda et al. for the fluidization and coat<strong>in</strong>g<br />
<strong>of</strong> very f<strong>in</strong>e particles. [75] In conventional fluidized-bed coat<strong>in</strong>g, whether<br />
it is top-spray, Wurster, or rotational, the basic concept <strong>of</strong> fluidization<br />
relies on the compensation <strong>of</strong> the gravitational force experienced by the<br />
particles by an upward mov<strong>in</strong>g air flow, which ensures complete fluidization<br />
<strong>of</strong> the particles. Typical fluidized-bed apparatus can efficiently<br />
process particles from 100 mm to a few millimeters. However, for very<br />
small particles, other forces, such as electrostatic forces, start to play<br />
a major role <strong>in</strong> the movement <strong>of</strong> the particles <strong>in</strong> the fluidization chamber<br />
and prevent adequate fluidization. Colloidal particles have been<br />
used with some success to reduce electrostatic force, but are not much<br />
help <strong>in</strong> the fluidization <strong>of</strong> very small (submicron) particles <strong>in</strong> a conventional<br />
fluidized-bed apparatus. In this <strong>in</strong>novative process (Fig. 6), however,<br />
the gravitational force is multiplied through the use <strong>of</strong> a rotat<strong>in</strong>g<br />
perforated drum that conta<strong>in</strong>s the particle. The air flow is then applied<br />
tangentially to the rotation <strong>of</strong> the drum as compensation for the gravitational<br />
force, now a multiple (up to 37 g) <strong>of</strong> the normal gravitational<br />
force.<br />
The conventional top-spray method rema<strong>in</strong>s unique and widely used<br />
technique <strong>in</strong> food <strong>in</strong>dustry. This is due to its high versatility, relatively high<br />
batch size, and relative simplicity. [75] <strong>Recent</strong>ly, cont<strong>in</strong>uous fluidized-bed<br />
Figure 6. Tangential-spray fluidized-bed coat<strong>in</strong>g.
1376 Desai and Park<br />
coaters have been developed. [76] With such a cont<strong>in</strong>uous fluidized-bed<br />
coat<strong>in</strong>g process, manufacturers can adapt the system to their own specific<br />
requirements while ma<strong>in</strong>ta<strong>in</strong><strong>in</strong>g the flexibility needed for a large material<br />
throughput and wide product ranges, and while provid<strong>in</strong>g the coat<strong>in</strong>g<br />
quality demanded <strong>in</strong> the food <strong>in</strong>dustry. The efficiency <strong>of</strong> fluidized-bed<br />
techniques is governed by process variables, ambient variables, and thermodynamic<br />
factors (Table 3). Appropriate modification or comb<strong>in</strong>ations<br />
<strong>of</strong> these variables will yield the desired results.<br />
The use <strong>of</strong> melted fats, waxes, or emulsifiers as shell materials is a<br />
relatively new but very promis<strong>in</strong>g and <strong>in</strong>terest<strong>in</strong>g concept. From an<br />
<strong>in</strong>dustrial po<strong>in</strong>t <strong>of</strong> view, the <strong>in</strong>herent advantage <strong>of</strong> hot-melt fluidizedbed<br />
coat<strong>in</strong>g lies <strong>in</strong> the fact that the coat<strong>in</strong>g formulation is concentrated<br />
(no solvent, as <strong>in</strong> aqueous-based coat<strong>in</strong>g formulation), which means<br />
dramatically shorter process<strong>in</strong>g times. The energy <strong>in</strong>put is also much<br />
lower than with aqueous-based formulation s<strong>in</strong>ce no evaporation needs<br />
to be done. Very few reports have been published on hot-melt coat<strong>in</strong>g<br />
by fluidized beds s<strong>in</strong>ce Jozwiakowsksi et al. described the coat<strong>in</strong>g <strong>of</strong><br />
sucrose particles with partially hydrogenated cottonseed oil and analyzed<br />
the optimal process<strong>in</strong>g parameters by modified central composite<br />
design. [77] A number <strong>of</strong> patent applications, very similar <strong>in</strong> process<strong>in</strong>g<br />
designs, have been published us<strong>in</strong>g fats and emulsifiers <strong>of</strong> various melt<strong>in</strong>g<br />
po<strong>in</strong>ts and have developed an <strong>in</strong>novative fluidized-bed process for coat<strong>in</strong>g<br />
particles with fats and waxes us<strong>in</strong>g supercritical carbon dioxide as the<br />
solvent for the coat<strong>in</strong>g formulation. [78–80] Here, aga<strong>in</strong>, m<strong>in</strong>imal energy<br />
<strong>in</strong>put is needed to evaporate the solvent and the process might lead to<br />
lower cost-<strong>in</strong>-use encapsulated <strong>in</strong>gredients.<br />
Table 3. Different variables <strong>in</strong>fluenc<strong>in</strong>g fluidized-bed operation<br />
No Variables<br />
1 Process variables<br />
1. Inlet air temperature<br />
2. Inlet air velocity<br />
3. Spray rate<br />
4. Solution temperature<br />
5. Solution dry matter content<br />
6. Atomization pressure<br />
2 Ambient variables<br />
1. Ambient air temperature<br />
2. Ambient air relative humidity<br />
3 Thermodynamic<br />
1. Outlet air temperature<br />
2. Outlet air relative humidity
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1377<br />
APPLICATION OF FLUIDIZED-BED TECHNIQUE<br />
IN FOOD INDUSTRY<br />
This technique is used to encapsulate nutritional substances such as<br />
vitam<strong>in</strong> C, B vitam<strong>in</strong>s, ferrous sulfate, ferrous fumarate, sodium ascorbate,<br />
potassium chloride, and a variety <strong>of</strong> vitam<strong>in</strong>=m<strong>in</strong>eral premixes.<br />
These encapsulated products are used as nutritional supplements. [81] In<br />
the case <strong>of</strong> bakery products, it is also used to encapsulate the leaven<strong>in</strong>g<br />
system <strong>in</strong>gredients, as well as vitam<strong>in</strong> C, acetic acid, lactic acid, potassium<br />
sorbate, sorbic acid, calcium propionate, and salt. [81,82] In the meat<br />
<strong>in</strong>dustry, several food acids have been fluid-bed encapsulated to develop<br />
color and flavor systems. They are also used to achieve a reproducible pH<br />
<strong>in</strong> cured meat products and to shorten their process<strong>in</strong>g time. Fluid-bed<br />
encapsulated salt is used <strong>in</strong> meats to prevent development <strong>of</strong> rancidity,<br />
as well as premature set due to my<strong>of</strong>ibrilar b<strong>in</strong>d<strong>in</strong>g. [81]<br />
Extrusion<br />
Encapsulation <strong>of</strong> food <strong>in</strong>gredients by extrusion is a relatively new process<br />
compared to spray-dry<strong>in</strong>g. Extrusion used <strong>in</strong> this context is not same as<br />
extrusion used for cook<strong>in</strong>g and texturiz<strong>in</strong>g <strong>of</strong> cereal-based products. Actually,<br />
extrusion, as applied to flavor encapsulation, is a relatively lowtemperature<br />
entrapp<strong>in</strong>g method, which <strong>in</strong>volves forc<strong>in</strong>g a core material <strong>in</strong><br />
a molten carbohydrate mass through a series <strong>of</strong> dies <strong>in</strong>to a bath <strong>of</strong> dehydrat<strong>in</strong>g<br />
liquid. The pressure and temperature employed are typically
1378 Desai and Park<br />
Figure 7. Flow diagram <strong>of</strong> encapsulation <strong>of</strong> food flavors by extrusion method.<br />
core material is removed from the surface <strong>in</strong> an alcohol bath. [14,51,71,81]<br />
This provides an excellent stability aga<strong>in</strong>st oxidation and therefore prolongs<br />
the shelf life. The product can be kept for 1–2 years without any<br />
substantial quality degradation. [71,81] This technique can be classified as<br />
a glass encapsulation system or a controlled-release system, depend<strong>in</strong>g<br />
on the polymeric materials used. The polymer matrices and the plasticizers<br />
used can be modified to produce the capsules for controlled release<br />
<strong>in</strong> food application. [85] However, microcapsules produced from this<br />
method are commonly designed to be soluble <strong>in</strong> water by the use <strong>of</strong><br />
high-molecular-weight hydrophilic polymer. Thus, this encapsulation<br />
technique is considered unsuitable for subsequent extrusion process<strong>in</strong>g<br />
because the water <strong>in</strong> the extruder melt can dissolve the capsules. [86]<br />
Centrifugal Extrusion<br />
Centrifugal extrusion is another encapsulation technique that has been<br />
<strong>in</strong>vestigated and used by some manufacturers. A number <strong>of</strong> food-approved
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1379<br />
coat<strong>in</strong>g systems have been formulated to encapsulate products such as<br />
flavor<strong>in</strong>gs, season<strong>in</strong>gs, and vitam<strong>in</strong>s. These wall materials <strong>in</strong>clude gelat<strong>in</strong>,<br />
sodium alg<strong>in</strong>ate, carrageenan, starches, cellulose derivatives, gum<br />
acacia, fats=fatty acids, waxes, and polyethylene glycol. Centrifugal<br />
extrusion is a liquid coextrusion process utiliz<strong>in</strong>g nozzles consist<strong>in</strong>g <strong>of</strong><br />
concentric orifice located on the outer circumference <strong>of</strong> a rotat<strong>in</strong>g cyl<strong>in</strong>der<br />
(i.e., head). The encapsulat<strong>in</strong>g cyl<strong>in</strong>der or head consists <strong>of</strong> a concentric<br />
feed tube through which coat<strong>in</strong>g and core materials are pumped<br />
separately to the many nozzles mounted on the outer surface <strong>of</strong> the<br />
device. While the core material passes through the center tube, coat<strong>in</strong>g<br />
material flows through the outer tube. The entire device is attached to a<br />
rotat<strong>in</strong>g shaft such that the head rotates around its vertical axis. As the<br />
head rotates, the core and coat<strong>in</strong>g materials are co-extruded through<br />
the concentric orifices <strong>of</strong> the nozzles as a fluid rod <strong>of</strong> the core sheathed<br />
<strong>in</strong> coat<strong>in</strong>g material. Centrifugal force impels the rod outward, caus<strong>in</strong>g it<br />
to break <strong>in</strong>to t<strong>in</strong>y particles. By the action <strong>of</strong> surface tension, the coat<strong>in</strong>g<br />
material envelops the core material, thus accomplish<strong>in</strong>g encapsulation.<br />
The microcapsules are collected on a mov<strong>in</strong>g bed <strong>of</strong> f<strong>in</strong>e-gra<strong>in</strong>ed starch,<br />
which cushions their impact and absorbs unwanted coat<strong>in</strong>g moisture.<br />
Particles produced by this method have diameter rang<strong>in</strong>g from 150 to<br />
2000 mm. [87]<br />
Lyophilization<br />
Lyophilization, or freeze-dry<strong>in</strong>g, is a process used for the dehydration <strong>of</strong><br />
almost all heat-sensitive materials and aromas. It has been used to encapsulate<br />
water-soluble essences and natural aromas as well as drugs. Except<br />
for the long dehydration period required (commonly 20 h), freeze-dry<strong>in</strong>g<br />
is a simple technique, which is particularly suitable for the encapsulation<br />
<strong>of</strong> aromatic materials. The retention <strong>of</strong> volatile compounds dur<strong>in</strong>g the<br />
lyophilization is dependent upon the chemical nature <strong>of</strong> the system. [88]<br />
Coacervation<br />
Coacervation <strong>in</strong>volves the separation <strong>of</strong> a liquid phase <strong>of</strong> coat<strong>in</strong>g<br />
material from a polymeric solution followed by the coat<strong>in</strong>g <strong>of</strong> that phase<br />
as a uniform layer around suspended core particles. The coat<strong>in</strong>g is then<br />
solidified. In general, the batch-type coacervation processes consist <strong>of</strong><br />
three steps and are carried out under cont<strong>in</strong>uous agitation.<br />
1. Formation <strong>of</strong> a three-immiscible chemical phase<br />
2. Deposition <strong>of</strong> the coat<strong>in</strong>g<br />
3. Solidification <strong>of</strong> the coat<strong>in</strong>g
1380 Desai and Park<br />
In the first step, a three-phase system consist<strong>in</strong>g <strong>of</strong> a liquid manufactur<strong>in</strong>g<br />
vehicle phase, a core material phase, and a coat<strong>in</strong>g material phase<br />
is formed by either a direct addition or <strong>in</strong> situ separation technique. In<br />
the direct addition approach, the coat<strong>in</strong>g-<strong>in</strong>soluble waxes, immiscible<br />
solutions, and <strong>in</strong>soluble liquid polymers are added directly to the<br />
liquid-manufactur<strong>in</strong>g vehicle, provided that it is immiscible with the<br />
other two phases and is capable <strong>of</strong> be<strong>in</strong>g liquefied. In the <strong>in</strong> situ separation<br />
technique, a monomer is dissolved <strong>in</strong> the liquid vehicle and is then<br />
subsequently polymerized at the <strong>in</strong>terface. Deposition <strong>of</strong> the liquid polymer<br />
coat<strong>in</strong>g around the core material is accomplished by controlled<br />
physical mix<strong>in</strong>g <strong>of</strong> the coat<strong>in</strong>g material (while liquid) and the core<br />
material <strong>in</strong> the manufactur<strong>in</strong>g vehicle <strong>in</strong> the liquid phase; this sorption<br />
phenomenon is a prerequisite to effective coat<strong>in</strong>g. Cont<strong>in</strong>ued deposition<br />
<strong>of</strong> the coat<strong>in</strong>g is prompted by a reduction <strong>in</strong> the total free <strong>in</strong>terfacial<br />
energy <strong>of</strong> the system brought about by a decrease <strong>of</strong> the coat<strong>in</strong>g material<br />
surface area dur<strong>in</strong>g coalescence <strong>of</strong> the liquid polymer droplets. F<strong>in</strong>ally,<br />
solidification <strong>of</strong> the coat<strong>in</strong>g is achieved by thermal, cross-l<strong>in</strong>k<strong>in</strong>g, or desolventization<br />
techniques and forms a self-susta<strong>in</strong><strong>in</strong>g microcapsule. The<br />
microcapsules are usually collected by filtration or centrifugation,<br />
washed with an appropriate solvent, and subsequently dried by standard<br />
techniques such as spray- or fluidized-bed dry<strong>in</strong>g to yield free-flow<strong>in</strong>g,<br />
discrete particles. [7]<br />
A large numbers <strong>of</strong> coat<strong>in</strong>g materials have been evaluated for coacervation<br />
microencapsulation but the most studied and well understood<br />
coat<strong>in</strong>g system is probably the gelat<strong>in</strong>=gum acacia system. However,<br />
other coat<strong>in</strong>g systems such as gliad<strong>in</strong>, hepar<strong>in</strong>=gelat<strong>in</strong>, carrageenan,<br />
chitosan, soy prote<strong>in</strong>, polyv<strong>in</strong>yl alcohol, gelat<strong>in</strong>=carboxymethylcellulose,<br />
B-lactoglobul<strong>in</strong>=gum acacia, and guar gum=dextran are also studied. [89]<br />
In recent years, modified coacervation processes have also been developed<br />
that can overcome some <strong>of</strong> the problems encountered dur<strong>in</strong>g a typical<br />
gelat<strong>in</strong>=gum acacia complex coacervation process, especially when deal<strong>in</strong>g<br />
with food <strong>in</strong>gredients; for example, a room-temperature process for the<br />
encapsulation <strong>of</strong> heat-sensitive <strong>in</strong>gredients such as volatile flavor oils. [90]<br />
In this process, the coat<strong>in</strong>g materials are mixed and then phase separation<br />
(coacervation) is achieved by adjust<strong>in</strong>g the pH. The newly formed coacervate<br />
phase is allowed to separate and sediment, most <strong>of</strong> the supernatant<br />
water is removed, and the flavor oil is then added to the mixture kept at<br />
50 C and emulsified rapidly. The <strong>in</strong>itial volume <strong>of</strong> water is restored with<br />
room temperature water, caus<strong>in</strong>g a quick drop <strong>in</strong> the temperature, which<br />
means that the flavor oils experience a high temperature for only a few<br />
m<strong>in</strong>utes, compared to several hours for a typical coacervation process.<br />
Another process <strong>in</strong>volves the formation <strong>of</strong> a multilayered coacervated<br />
microcapsule. [91] This process consists <strong>of</strong> multiple coacervation stages <strong>in</strong><br />
which an additional layer <strong>of</strong> wall material is applied to the microcapsule<br />
at each passage and the f<strong>in</strong>al shell layer can reach a thickness up to 100 mm.
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1381<br />
The coacervation method has some drawbacks. This process is very<br />
expensive and rather complex, and cross-l<strong>in</strong>k<strong>in</strong>g <strong>of</strong> the wall material<br />
usually <strong>in</strong>volves glutaraldehyde, which must be carefully used accord<strong>in</strong>g<br />
to the country’s legislation. The problems related to harmful chemical<br />
cross-l<strong>in</strong>kers could eventually be solved by us<strong>in</strong>g enzymatic cross-l<strong>in</strong>kers<br />
<strong>in</strong>stead. Soper and Thomas, for <strong>in</strong>stance, described a process <strong>in</strong> which a<br />
transglutam<strong>in</strong>ase is used to cross-l<strong>in</strong>k the prote<strong>in</strong>s <strong>in</strong> the shell material.<br />
The enzyme is added to the microencapsulation tank at 10 C and pH 7<br />
and the reaction is carried out over 16 h, after which a hardened shell<br />
<strong>of</strong> coacervate is formed around the flavor oil droplets. [92]<br />
Centrifugal Suspension Separation<br />
Centrifugal suspension is more recent microencapsulation process. The<br />
process <strong>in</strong> pr<strong>in</strong>ciple <strong>in</strong>volves mix<strong>in</strong>g the core and wall materials and then<br />
add<strong>in</strong>g to a rotat<strong>in</strong>g disk. The core materials then leave the disk with a<br />
coat<strong>in</strong>g <strong>of</strong> residual liquid. The microcapsules are then dried or chilled<br />
after removal from the disk. The whole process can take between a few<br />
seconds to m<strong>in</strong>utes. Solids, liquids, or suspensions <strong>of</strong> 30 mm to2mm<br />
can be encapsulated <strong>in</strong> this manner. Coat<strong>in</strong>gs can be 1–200 mm <strong>in</strong> thickness<br />
and <strong>in</strong>clude fats, polyethylene glycol (PEG), diglycerides, and other<br />
meltable substances. S<strong>in</strong>ce this is a cont<strong>in</strong>uous, high-speed method that<br />
can coat particles, it is highly suitable for foods. One application is to<br />
protect foods that are sensitive to or readily absorb moisture, such as<br />
aspartame, vitam<strong>in</strong>s, or methion<strong>in</strong>e. [93] The preparation process <strong>of</strong> encapsulated<br />
particles by centrifugal suspension separation is illustrated <strong>in</strong><br />
Fig. 8.<br />
Cocrystallization<br />
Cocrystallization is a new encapsulation process utiliz<strong>in</strong>g sucrose as a<br />
matrix for the <strong>in</strong>corporation <strong>of</strong> core materials. The sucrose syrup is concentrated<br />
to the supersaturated state and ma<strong>in</strong>ta<strong>in</strong>ed at a temperature<br />
high enough to prevent crystallization. A predeterm<strong>in</strong>ed amount <strong>of</strong> core<br />
material is then added to the concentrated syrup with vigorous mechanical<br />
agitation, thus provid<strong>in</strong>g nucleation for the sucrose=<strong>in</strong>gredient mixture<br />
to crystallize. As the syrup reaches the temperature at which transformation<br />
and crystallization beg<strong>in</strong>, a substantial amount <strong>of</strong> heat is emitted.<br />
Agitation is cont<strong>in</strong>ued <strong>in</strong> order to promote and extend transformation=<br />
crystallization until the agglomerates are discharged from the vessel.<br />
The encapsulated products are then dried to the desired moisture (if<br />
necessary) and screened to a uniform size. It is very important to properly<br />
control the rates <strong>of</strong> nucleation and crystallization as well as the thermal<br />
balance dur<strong>in</strong>g the various phases. [94]
1382 Desai and Park<br />
Figure 8. Representation <strong>of</strong> rotational suspension separation (A: establish<strong>in</strong>g<br />
particle size for pure coat<strong>in</strong>g, and B: encapsulation by suspension separation).<br />
The advantages <strong>of</strong> this technique <strong>in</strong>clude: (1) It can be employed to<br />
achieve particle dry<strong>in</strong>g. By means <strong>of</strong> this process, core materials <strong>in</strong> a<br />
liquid form can be converted to a dry powdered form without additional<br />
dry<strong>in</strong>g. (2) Products <strong>of</strong>fer direct tablet<strong>in</strong>g characteristics because <strong>of</strong> their<br />
agglomerated structure and thus <strong>of</strong>fer significant advantages to the candy<br />
and pharmaceutical <strong>in</strong>dustries. <strong>Recent</strong>ly, Berista<strong>in</strong> et al. encapsulated<br />
orange peel oil by a cocrystallization technique. [95] In their study, encapsulation<br />
capacity <strong>of</strong> sucrose syrups was found to be greater than 90% for<br />
a range <strong>of</strong> 100 to 250 g oil=kg <strong>of</strong> sugar. Surface oil, a measurement <strong>of</strong><br />
encapsulation efficiency, varied from 3350 to 8880 mg oil=kg solids.<br />
Moisture content <strong>of</strong> the crystals was lower than 10 g=kg, and bulk density<br />
was greater than 670 kg=m 3 for all the cocrystallizates prepared. Sensory<br />
evaluation showed that all <strong>of</strong> the panelists were able to detect oxidized<br />
flavors <strong>in</strong> oils without antioxidant added after storage at 35 C for one<br />
day. When butylated hydroxyanisole was added to the oil prior to cocrystallization,<br />
no signs <strong>of</strong> oxidized flavors were detected after 2 months <strong>of</strong><br />
storage at ambient temperature.<br />
Liposome Entrapment<br />
Liposomes consist <strong>of</strong> an aqueous phase that is completely surrounded by<br />
a phospholipid-based membrane. When phospholipids, such as lecith<strong>in</strong>,
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1383<br />
are dispersed <strong>in</strong> an aqueous phase, the liposomes form spontaneously.<br />
One can have either aqueous or lipid-soluble material enclosed <strong>in</strong> the<br />
liposome. They have been used for delivery <strong>of</strong> vacc<strong>in</strong>es, hormones,<br />
enzymes, and vitam<strong>in</strong>s. [96] They consist <strong>of</strong> one or more layers <strong>of</strong> lipids<br />
and thus are nontoxic and acceptable for foods. Permeability, stability,<br />
surface activity, and aff<strong>in</strong>ity can be varied through size and lipid composition<br />
variations. They can range from 25 nm to several microns <strong>in</strong> diameter,<br />
are easy to make, and can be stored by freeze-dry<strong>in</strong>g. Kirby and<br />
Gregoriadis have devised a method to encapsulate at high efficiency,<br />
which is easy to scale-up and uses mild conditions appropriate for<br />
enzymes. [97] It is important to reiterate that large unilamellar vesicles<br />
(LUV) are the most appropriate liposomes for the food <strong>in</strong>dustry because<br />
<strong>of</strong> their high encapsulation efficiency, their simple production methods,<br />
and their good stability over time. The great advantage <strong>of</strong> liposomes over<br />
other microencapsulation technologies is the stability liposomes impart<br />
to water-soluble material <strong>in</strong> high water activity application: spray-dryers,<br />
extruders, and fluidized beds impart great stability to food <strong>in</strong>gredients <strong>in</strong><br />
the dry state but release their content readily <strong>in</strong> high water activity application,<br />
giv<strong>in</strong>g up all protection properties. Another unique property <strong>of</strong><br />
liposomes is the targeted delivery <strong>of</strong> their content <strong>in</strong> specific parts <strong>of</strong> the<br />
foodstuff. For example, it has been shown that liposome-encapsulated<br />
enzymes concentrate preferably <strong>in</strong> the curd dur<strong>in</strong>g cheese formation,<br />
whereas nonencapsulated enzymes are usually distributed evenly <strong>in</strong> the<br />
whole milk mixture, which leads to very low (2–4%) retention <strong>of</strong> the<br />
flavor-produc<strong>in</strong>g enzymes <strong>in</strong> the curd. They have prepared bromela<strong>in</strong>loaded<br />
liposomes for use as meat-tenderizer to improve stability <strong>of</strong><br />
the enzyme dur<strong>in</strong>g the process<strong>in</strong>g <strong>of</strong> the food and subsequently improve<br />
the availability <strong>of</strong> the enzyme. [98] Benech Kheadr et al. showed that<br />
liposome-entrapped nis<strong>in</strong> reta<strong>in</strong>ed higher activity aga<strong>in</strong>st Listeria <strong>in</strong>nocua<br />
and had improved stability <strong>in</strong> cheese production, prov<strong>in</strong>g a powerful<br />
tool to <strong>in</strong>hibit the growth <strong>of</strong> Listeria I <strong>in</strong> cheese while not prevent<strong>in</strong>g<br />
the detrimental effect <strong>of</strong> nis<strong>in</strong> on the actual cheese-ripen<strong>in</strong>g process. [99]<br />
Kirby et al. have developed a process to stabilize vitam<strong>in</strong> C <strong>in</strong> the aqueous<br />
<strong>in</strong>ner core <strong>of</strong> liposomes. [100] Encapsulation <strong>of</strong> vitam<strong>in</strong> C gave significant<br />
improvements <strong>in</strong> shelf life (from a few days to up to 2 months),<br />
especially <strong>in</strong> the presence <strong>of</strong> common food components that would normally<br />
speed up decomposition, such as copper ions, ascorbate oxidase,<br />
and lys<strong>in</strong>e. Liposomes can also be used to deliver the encapsulated<br />
<strong>in</strong>gredient at a specific and well-def<strong>in</strong>ed temperature: the liposome<br />
bilayer is <strong>in</strong>stantly broken down at the transition temperature <strong>of</strong> the<br />
phospholipids, typically around 50 C, at which temperature the content<br />
is immediately released.<br />
The most common phospholipid <strong>in</strong> lect<strong>in</strong>, phosphatidyl chol<strong>in</strong>e, is<br />
<strong>in</strong>soluble <strong>in</strong> water and is <strong>in</strong>expensively isolated from soy or egg yolk.<br />
The composition <strong>of</strong> the phospholipids and the process used determ<strong>in</strong>e
1384 Desai and Park<br />
if a s<strong>in</strong>gle layer or multiple layers are formed. Fatty acids also make up<br />
liposomes and their degree <strong>of</strong> saturation is dependent on the source. Animal<br />
sources provide more saturated fatty acids. They <strong>in</strong>fluence the transition<br />
temperature, which is the conversion from a gel to the more leaky<br />
liquid form. The ma<strong>in</strong> issues <strong>in</strong> liposome encapsulation for the food<br />
<strong>in</strong>dustry are (1) the scal<strong>in</strong>g up <strong>of</strong> the microencapsulation process at<br />
acceptable cost-<strong>in</strong>-use levels and (2) the delivery form <strong>of</strong> the liposomeencapsulated<br />
<strong>in</strong>gredients. The development <strong>of</strong> a cost-effective dry<strong>in</strong>g<br />
method for liposome microcapsules and development <strong>of</strong> a dry liposome<br />
formulation that readily reconstitutes upon rehydration would ensure<br />
a promis<strong>in</strong>g future to liposome encapsulation <strong>of</strong> food <strong>in</strong>gredients. The<br />
recent advances <strong>in</strong> liposome technology have most probably solved<br />
the first issue: micr<strong>of</strong>luidization has been shown to be an effective,<br />
cost-effective, and solvent-free cont<strong>in</strong>uous method for the production<br />
<strong>of</strong> liposomes with high encapsulation efficiency. The method can process<br />
a few hundred liters per hour <strong>of</strong> aqueous liposomes on a cont<strong>in</strong>uous<br />
basis. [101,102] The other issue concerns the aqueous form <strong>in</strong> which the liposomes<br />
are usually delivered. Most <strong>of</strong> the time, if not always, liposome formulations<br />
are kept <strong>in</strong> relatively dilute aqueous suspensions and this might<br />
be a very serious drawback for the large-scale production, storage, and<br />
shipp<strong>in</strong>g <strong>of</strong> encapsulated food <strong>in</strong>gredients.<br />
Inclusion Complexation<br />
Molecular <strong>in</strong>clusion is another means <strong>of</strong> achiev<strong>in</strong>g encapsulation. Unlike<br />
other processes discussed to this po<strong>in</strong>t, this technique takes place at a<br />
molecular level; b-cyclodextr<strong>in</strong> is typically used as the encapsulat<strong>in</strong>g<br />
medium. b-Cyclodextr<strong>in</strong> is a cyclic derivative <strong>of</strong> starch made up <strong>of</strong> seven<br />
glucopyranose units. They are prepared from partially hydrolyzed starch<br />
(maltodextr<strong>in</strong>) by an enzymatic process. The external part <strong>of</strong> the cyclodextr<strong>in</strong><br />
molecule is hydrophilic, whereas the <strong>in</strong>ternal part is hydrophobic.<br />
The guest molecules, which are apolar, can be entrapped <strong>in</strong>to the apolar<br />
<strong>in</strong>ternal cavity through a hydrophobic <strong>in</strong>teraction. [103] This <strong>in</strong>ternal<br />
cavity <strong>of</strong> about 0.65 nm diameter permits the <strong>in</strong>clusion <strong>of</strong> essential oil<br />
compounds and can take up one or more flavor volatile molecules. [13]<br />
In this method, the flavor compounds are entrapped <strong>in</strong>side the hollow<br />
center <strong>of</strong> a b-cyclodextr<strong>in</strong> molecule. The chemical structure and geometry<br />
<strong>of</strong> b-cyclodextr<strong>in</strong> are shown <strong>in</strong> Fig. 9.<br />
b-Cyclodextr<strong>in</strong> molecules form <strong>in</strong>clusion complexes with compounds<br />
that can fit dimensionally <strong>in</strong>to their central cavity. These complexes are<br />
formed <strong>in</strong> a reaction that takes place only <strong>in</strong> the presence <strong>of</strong> water. Molecules<br />
that are less polar than water (i.e., most flavor substances) and have<br />
suitable molecular dimensions to fit <strong>in</strong>side the cyclodextr<strong>in</strong> <strong>in</strong>terior can<br />
be <strong>in</strong>corporated <strong>in</strong>to the molecule. There are three methods to produce
<strong>Microencapsulation</strong> <strong>of</strong> <strong>Food</strong> <strong>Ingredients</strong> 1385<br />
Figure 9. Molecular structure and microstructure <strong>of</strong> b-cyclodextr<strong>in</strong>. [79]<br />
the flavor-b-cyclodextr<strong>in</strong> complex. In the first method, b-cyclodextr<strong>in</strong> is<br />
dissolved <strong>in</strong> water to form an aqueous solution, and the flavors are added<br />
to form an <strong>in</strong>clusion complex <strong>in</strong> crystall<strong>in</strong>e form. The crystal obta<strong>in</strong>ed<br />
is then separated and dried. In the second method, b-cyclodextr<strong>in</strong> is<br />
dissolved <strong>in</strong> a lesser amount <strong>of</strong> water than <strong>in</strong> the first method to form<br />
a concentrated suspension, and the flavors are mixed to form an <strong>in</strong>clusion<br />
complex <strong>in</strong> crystall<strong>in</strong>e form. The complex then must be separated and<br />
dried. In the third method, b-cyclodextr<strong>in</strong> is dissolved <strong>in</strong> a much<br />
lower water content to form a paste, and the flavors are mixed dur<strong>in</strong>g<br />
knead<strong>in</strong>g to form an <strong>in</strong>clusion complex. This method is superior to the<br />
former two because it does not require further separation and dry<strong>in</strong>g. [103]<br />
A cyclodextr<strong>in</strong>-complexation method has been patented us<strong>in</strong>g a ball mill<br />
with a charge <strong>of</strong> cyclodextr<strong>in</strong> and a guest molecule. This process needs<br />
little water, preferably 25–60% moisture by weight. The <strong>in</strong>clusion<br />
capacity <strong>of</strong> 1 g <strong>of</strong> b-cyclodextr<strong>in</strong> is not more than 97 mg <strong>of</strong> lemon oil.<br />
Among all exist<strong>in</strong>g microencapsulation methods, molecular <strong>in</strong>clusion<br />
<strong>of</strong> flavor volatiles <strong>in</strong> b-cyclodextr<strong>in</strong> molecules is the most effective for<br />
protect<strong>in</strong>g the aromas. Encapsulat<strong>in</strong>g flavors <strong>in</strong> this way can provide<br />
better protection from volatilization dur<strong>in</strong>g extrusion. However, the use<br />
<strong>of</strong> b-cyclodextr<strong>in</strong> for food application is very limited, possibly due to<br />
regulatory requirements <strong>in</strong> a number <strong>of</strong> countries. [86]
1386<br />
Table 4. Encapsulated food <strong>in</strong>gredients and their application <strong>in</strong> food <strong>in</strong>dustry<br />
Preferred mode <strong>of</strong><br />
encapsulation Applications<br />
Category <strong>of</strong> food<br />
<strong>in</strong>gredients Examples<br />
No.<br />
1. Used to assist <strong>in</strong> the development<br />
<strong>of</strong> color and flavor <strong>in</strong> meat emulsions,<br />
dry sausage products, uncooked<br />
processed meats, and meat conta<strong>in</strong><strong>in</strong>g<br />
products.<br />
2. Bak<strong>in</strong>g <strong>in</strong>dustry use stable acids and<br />
bak<strong>in</strong>g soda <strong>in</strong> wet and dry mixes to<br />
control the release <strong>of</strong> carbon dioxide<br />
dur<strong>in</strong>g process<strong>in</strong>g and subsequent<br />
Fluidized-bed coat<strong>in</strong>g,<br />
extrusion<br />
1 Acidulants Lactic acid, glucono-d-lactone,<br />
vitam<strong>in</strong> C, acetic acid,<br />
potassium sorbate, sorbic acid,<br />
calcium propionate,<br />
and sodium chloride<br />
bak<strong>in</strong>g.<br />
1. To transform liquid flavor<strong>in</strong>gs <strong>in</strong>to<br />
stable and free flow<strong>in</strong>g powders, which<br />
are easier to handle and <strong>in</strong>corporate<br />
<strong>in</strong>to a dry food system.<br />
Inclusion complexation,<br />
extrusion, centrifugal<br />
extrusion, spray-dry<strong>in</strong>g<br />
2 Flavor<strong>in</strong>g agents Citrus oil, m<strong>in</strong>t oils,<br />
onion oils, garlic oils,<br />
spice oleores<strong>in</strong>s
3 Sweeteners Sugars, nutritive<br />
Cocrystallization,<br />
1. To reduce the hygroscopicity, improve<br />
or artificial sugars:<br />
fluidized-bed coat<strong>in</strong>g flowability, and prolong sweetness<br />
aspartame<br />
perception.<br />
4 Colorants Annatto, b-carotene, turmeric Extrusion, emulsion 1. Encapsulated colors are easier to<br />
handle and <strong>of</strong>fer improved solubility,<br />
stability to oxidation, and control<br />
over stratification from dry blends.<br />
5 Lipids Fish oil, l<strong>in</strong>olenic acid,<br />
Spray-dry<strong>in</strong>g, freeze-dry<strong>in</strong>g, 1. To prevent oxidative degradation<br />
rice bra<strong>in</strong> oil,<br />
vacuum-dry<strong>in</strong>g<br />
dur<strong>in</strong>g process<strong>in</strong>g and storage.<br />
egg white powder,<br />
sard<strong>in</strong>e oil,<br />
palmitic acid,<br />
1. To reduce <strong>of</strong>f-flavors.<br />
2. To permit time-release <strong>of</strong> nutrients.<br />
3. To enhance the stability to extremes <strong>in</strong><br />
temperature and moisture.<br />
4. To reduce each nutrient <strong>in</strong>teraction<br />
Coacervation,<br />
<strong>in</strong>clusion complexation,<br />
spray-dry<strong>in</strong>g,<br />
liposome entrapment<br />
seal blubber oil<br />
Fat-soluble:<br />
vitam<strong>in</strong> A, D, E, and K.<br />
Water-soluble: vitam<strong>in</strong> C,<br />
vitam<strong>in</strong> B1, vitam<strong>in</strong> B2,<br />
vitam<strong>in</strong> B6, vitam<strong>in</strong> B12,<br />
niac<strong>in</strong>, folic acid<br />
Lipase, <strong>in</strong>vertase,<br />
Brevibacterium l<strong>in</strong>ens,<br />
Penicillium roqueforti<br />
6 Vitam<strong>in</strong>s and<br />
m<strong>in</strong>erals<br />
other <strong>in</strong>gredients.<br />
1. To improve the stability.<br />
2. To reduce the ripen<strong>in</strong>g time.<br />
Coacervation,<br />
spray method,<br />
liposome entrapment<br />
7 Enzymes and<br />
microorganisms<br />
1387
1388 Desai and Park<br />
ENCAPSULATED INGREDIENTS AND APPLICATIONS<br />
<strong>Microencapsulation</strong> can potentially <strong>of</strong>fer numerous benefits to the materials<br />
be<strong>in</strong>g encapsulated. Various properties <strong>of</strong> active agents may be<br />
changed by encapsulation. For example, handl<strong>in</strong>g and flow properties<br />
can be improved by convert<strong>in</strong>g liquid to a solid encapsulated from.<br />
Hygroscopic materials can be protected from moisture. Some <strong>of</strong> the<br />
encapsulated food <strong>in</strong>gredients and their applications are summarized <strong>in</strong><br />
Table 4.<br />
CONCLUSIONS<br />
The use <strong>of</strong> microencapsulated food <strong>in</strong>gredients for controlled-release<br />
applications is a promis<strong>in</strong>g alternative to solve the major problem <strong>of</strong> food<br />
<strong>in</strong>gredients faced by food <strong>in</strong>dustries. The challenges are to select the<br />
appropriate microencapsulation technique and encapsulat<strong>in</strong>g material.<br />
Despite the wide range <strong>of</strong> encapsulated products that have been<br />
developed, manufactured, and successfully marketed <strong>in</strong> the pharmaceutical<br />
and cosmetic <strong>in</strong>dustries, microencapsulation has found a comparatively<br />
much smaller market <strong>in</strong> the food <strong>in</strong>dustry. The technology is still<br />
far from be<strong>in</strong>g fully developed and has yet to become a conventional tool<br />
<strong>in</strong> the food technologist’s repertoire for several reasons. First <strong>of</strong> all,<br />
the development time is rather long and requires multidiscipl<strong>in</strong>ary<br />
cooperation. Secondly, the low marg<strong>in</strong>s typically achieved <strong>in</strong> food <strong>in</strong>gredients<br />
and the relative <strong>in</strong>ertia <strong>of</strong> well-established corporations are an<br />
effective deterrent to the development and implementation <strong>of</strong> novel technologies<br />
that could result <strong>in</strong> truly unique food products, whether for<br />
more effective production, food fortification, neutraceuticals, improved<br />
organoleptic properties, or development <strong>of</strong> novelty food products. However,<br />
the most important aspect <strong>of</strong> R&D, from the very first lab-bench<br />
tests, is an understand<strong>in</strong>g <strong>of</strong> the <strong>in</strong>dustrial constra<strong>in</strong>ts and requirements<br />
to make a microencapsulation process viable, from the transition to<br />
full-scale production to the market<strong>in</strong>g <strong>of</strong> the f<strong>in</strong>al product.<br />
ACKNOWLEDGEMENT<br />
This study was supported by a grant <strong>of</strong> the Korea Health 21 R and D<br />
Project, M<strong>in</strong>istry <strong>of</strong> Health and Welfare, Republic <strong>of</strong> Korea (A050376).<br />
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