1 s2.0 S2667025922000206 Main
1 s2.0 S2667025922000206 Main
1 s2.0 S2667025922000206 Main
a r t i c l e i n f o a b s t r a c t
Keywords: Food colloids are mounting curiosity in the food industry to meet modern demands and challenges. The food
Hydrogel beads hydrocolloids market was valued at approximately USD 9928.5 million in 2021 and expected to increase to
Functional food approximately USD 13,381.3 million by 2028. Colloidal delivery systems, particularly hydrogel beads, are in-
Active delivery
tensely focused on sustainability, health wellbeing, and sensory perceptions.x Around 23,500 research articles on
Future food
hydrogel beads have been published in the previous ten years. The successful incorporation of gel beads into the
human food system requires an in-depth understanding of beads’ production, properties, release, or dissociation
mechanisms at different targeted sites. This review has pointed out the latest developments and achievements
in hydrogel beads from micro to millimeter-scale in the food industry. Various techniques for systematically
producing different kinds of gel beads were also summarized. The fundamental properties and mechanisms of
polysaccharides and protein-based materials that can be used for fabricating hydrogel beads are presented with
examples. Designing gel beads is a complicated and elusive process where numerous factors must be considered.
Apart from gel beads’ functional properties, sensory perception is also a fundamental consideration in formulating
gel beads for the human food system. The articleended with the potential future prospect of hydrogel beads. Gel
beads are still predominantly on a laboratory scale, with a high potential to flourish in the future food system.
This will provide a comprehensive idea of the fascinating field of hydrogel beads with up-to-date information.
∗
Corresponding author at: School of Food Science and Technology, Jiangnan University, Wuxi 214122, China
E-mail address: fzhong@jiangnan.edu.cn (F. Zhong).
https://doi.org/10.1016/j.fhfh.2022.100073
Received 31 March 2022; Received in revised form 28 May 2022; Accepted 3 June 2022
2667-0259/© 2022 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/)
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Since the beginning of the twenty-first century, an upsurge in scien- The design and development of such a colloidal system required an in-
tific achievement and industrial production, both in quantity and diver- depth understanding of binding and release mechanisms for a particu-
sity, has been noted regarding the encapsulation of various compounds lar compound in a specific system. This review was focused on gath-
in the food system (Thies, 2012; Timilsena, Haque, & Adhikari, 2020). ering up-to-date information about the formation, release, and signifi-
The global probiotics market was valued at USD 58.17 billion and was cance of hydrogel beads from the perspective of the future food system.
expected to grow around 7.5% from 2021 to 2030. While Omega-3, vita- Commonly used hydrogels, including both polysaccharides and protein,
min supplements, botanical supplements, seaweed, pre-biotics, and nu- are described with their physicochemical properties relating to hydrogel
traceuticals are reported to have an 8.2%, 6.2%, 9.1%, 10.8%, 6.6%, beads. Their gelling mechanism and bead forming properties will also
and 10.1% increase respectively in the next ten years of time. Surpris- be described considering various delivery systems.
ingly, insect protein outnumbered all other common health products,
with a forecast of a 27.4% increase over the 2021-2028 time period
(Grand View Research, 2022). The food colloids market was nearly 10 2. Why hydrogel beads?
million in 2021, with forcasted growth of 5.1% by 2028 (Zion Market
Research, 2022). This indicated the upcoming changes in global con- The concept of encapsulation has evolved in food science since many
sumer consciousness about healthy lifestyles and food habits. food components cannot be used as a direct additive due to poor stability
Furthermore, in today’s world, people are becoming busier by the or adverse sensory impact. Again, some functional components also need
day, leaving them with little time to prepare a healthy meal. As a result, to reach the targeted site, overcoming the harsh digestive environment.
a minimal process with functional, healthy food components is gaining At the same time, some components needed to be modified for prolonged
attraction. Again, due to globalization, humans’ tastes and choices for storage or transport convenience. Colloidal particulates lead the concept
innovative food textures and appearances are changing at such an ac- of encapsulation to an advanced level. Gel beads can be preferential over
celerated rate that food manufacturers are challenged every now and some conventional systems considering the following issues:
then to meet the demand. One of the promising practices is utilizing a Safety: The first and foremost condition of a food system is that it has
colloidal particulate system in the food industry. to be safe. Hydrogel beads are generally prepared from natural food col-
Hydrogels are three-dimensional colloidal systems composed of loids. Thus, they are safe and usually do not interfere with the trapped
physically or chemically associated linear or branched polymer chains component. Again, a reactive or incompatible component can be eas-
that contain a large quantity of water or biological fluid. Hydrogels ily removed. With only a few exceptions, most of the biomaterials that
can be composed of homogenous or heterogeneous materials and can are used for hydrogel beads are biocompatible, non-toxic, and certified
be designed to achieve tuned mechanical and physicochemical proper- as GRAS (generally recognized as safe) (Franco, Tommasina, & Pietro,
ties. Hydrogels have been promising in biomedical and food applica- 2016; Goff & Guo, 2020).
tions because of their bioavailability, bio-computability, tunable chemi- Attractive: After ensuring safety, the next things that come to the
cal or physical characteristics, non-toxic nature, and flexible fabrication mind of a consumer are the attractive texture and taste. In this regard,
(Maitra & Shukla, 2014; Redaelli, Sorbona, & Rossi, 2017). hydrogel beads are an odds-on-favorite. It can be customized to any
The circular or spherical shape is omnipresent in nature. Curvilinear desired texture, size, shape, or color. It has all the potential to draw the
shapes are more appealing to humans (Bar & Neta, 2007). It applies to attention of consumers of all ages (Stribiţcaia, Krop, Lewin, Holmes, &
our eating behavior as well. Fruits, foods, cakes, chocolate, and even Sarkar, 2020; Zegler, 2018).
eating plates and tables are all round. All these are subliminal factors Specific requirements: Since food production has to be considered
but play a significant role in humans’ minds perceiving food. Our brain globally now, a specific requirement like "Halal" or "Kosher" needs to
automatically associates round shape foods and sweet foods as safe, gen- be fulfilled. Most hydrogel beads are made from a wide range of nat-
tle, pleasant, graceful, dreamy, and even beautiful shapes that evoke ural biopolymers that can easily meet these regulations. In addition,
calmness, peacefulness, and relaxation. The circle’s inescapable beauty dietary or safety regulations are also not a major concern since most of
seems deeply rooted in our biology (Lima, 2017). these materials are already approved globally (Seisun & Zalesny, 2021;
A food hydrogel bead can be defined as a spherical complex three- Thies, 2012).
dimensional colloidal system where active materials can be dispersed Targeted delivery: Hydrogels can easily be designed for a targeted
or embodied in the core surrounded by a continuous protective shell. delivery path like the mouth, stomach, intestine, or colon. Beads can be
Gel beads may have multitudinous internal or external structures de- fabricated to sustain different digestive environments (Li et al., 2021;
pending on their purpose. In the modern food system, there are many Wong et al., 2021).
promising aspects of gel beads, as they can effectively resolve myriad Easy fabrication: Although some bead manufacturing requires spe-
challenges; such as their ability to be incorporated into the food ma- cific and sophisticated instrumentation, most gel beads are made with-
trix without compromising quality; their potential to protect functional out the use of expensive or high-tech equipment or processes. Regular
compounds from chemical, physical, or biological degradation; mask food processing technologies can be applied to make beads with versa-
off-flavors; deliver them to a specific site-of-action where they exhibit tile encapsulants (Li et al., 2021).
activity; improve storage, handling, and utilization; and extend shelf Diversified: The same gel beads can be designed to carry diversified
life. Numerous compounds have already been reported to be trapped materials. The system can efficiently encapsulate both small and large
and transported through gel beads incorporated into foods (Banerjee molecules (Wong et al., 2021).
& Bhattacharya, 2012; Li et al., 2022;Maleki, Woltering, & Mozafari, Controllable delivery: The release of materials from gel beads can
2022). Aside from their functionality, they can also produce appeal- easily be controlled. Delivery like intestinal absorption requires slow,
ing textures with exciting mouthfeels (Saqib, Ahammed, Liu, & Zhong, prolonged delivery, while flavor requires quick release in the mouth
2022). Gel beads have also been reported to be an absorbent for harmful (Mackie, 2012).
chemical compounds (Karimi & Namazi, 2022). In addition, advanced Survivability: Beads can protect active materials during processing,
materials and processes (e.g., coating, composite materials, etc.) can be cooking, or in a harsh stomach environment.Bioactive compounds can
used to create mechanically robust beads that overcome the biomate- be protected from the harsh external environment by improving the
rial’s poor mechanical properties (Lai, Wong, & Wong, 2020). Therefore, bioavailability of orally administered molecules within the hydrogel ma-
spherical gel beads have made provisions with great potential in food trix (Corstens et al., 2017; . Guo et al., 2017).
design. Transport and storage: Gel beads are simple to transport and store
These active compounds can then be designed to be delivered to because they are mechanically sound enough to keep their shape and
a particular targeted site like the mouth, stomach, intestine, or colon. are no longer distinguishable from regular foods.
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Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
3. Materials for bead production years (Delrieu & Ding, 2001; Huag & Draget, 2017; Sharma, Sharma, &
Majumdar, 2014).
Certain biopolymers are suitable for the entrapment of bioactive
compounds, considering the environment of the release site in the 3.1.4. Chitosan
gastro-intestinal tract. Sometimes these biopolymers are used in com- Chitosan is extracted commercially from the shells of shrimp and
binations of two or more, depending on their operational nature. Agar, other sea crustaceans. It is a positively charged polysaccharide typically
alginate, chitosan, cellulose, carrageenan, and bound proteins (e.g. col- used to coat bioactive compounds in previously formed encapsulation
lagen, gelatin, egg white) are the familiar biopolymer sources used to systems, such as probiotics encapsulated in an alginate matrix. An ad-
make hydrogel beads. This review segment will enumerate the available ditional chitosan coating provides better protection until it reaches the
resources for producing hydrogel beads—a summary of the available targeted destination in the GI tract (Reque & Brandelli, 2021). Chitosan
materials with their functionality tabulated in Table 1 (improvised with is an excellent excipient because it is non-toxic, stable, biodegradable,
permission from (Banerjee & Bhattacharya, 2012). and sterilized. These properties also make chitosan a versatile mate-
rial with extensive application in the biomedical and biotechnological
3.1. Polysaccharide-based materials fields (Kumar, Muzzarelli, Muzzarelli, Sashiwa, & Domb, 2004). As a
cationic polysaccharide, chitosan is extensively used in crosslinking, es-
3.1.1. Alginate pecially with alginate or other anionic substances, to make different
Alginate is the most widely used food colloid that has been utilized to types of hydrogel beads. In addition, chitosan can provide excellent me-
prepare beads. It is a heterogenic anionic polymer mainly extracted from chanical and structural stability for gel beads (Fei, Yang, Xie and Zheng,
brown seaweed. A few species of Azotobacter and Pseudomonas were also 2018;Maleki, Woltering and Mozafari, 2022; Puguan, Yu, & Kim, 2014).
reported to produce alginate (Nordgård & Draget, 2021). The most inter-
esting and unique properties of alginate that give it versatile properties 3.1.5. Cellulose
are that it can produce mechanically stable, thermo-irreversible gels in Cellulose is renowned for its biocompatibility, biodegradability, re-
the presence of cation. The crosslinked gel is a two- or three-dimensional newability, good mechanical strength, environmental friendliness, and
hydrophilic polymeric network that can hold a huge amount of bio- being one of the safest materials on earth. For these reasons, cellu-
logical fluid (Gudmund Skjak-Bræk, Ivan Donati, 2016). Alginate-based lose is extensively used as a coating material in encapsulating bioac-
hydrogel beads can be designed in different forms, such as nanopar- tive compounds (Ergun, Guo, & Huebner-Keese, 2016). To prepare hy-
ticles, microparticles, solid hydrogel, emulsion-filled beads, emulsions, drogel beads from cellulose and its derivatives, chemical crosslinking,
core-shell particles, liposomes, aerogels, etc. (Ching, Bansal, & Bhan- physical crosslinking or polymerization techniques, or a combination of
dari, 2017; Hariyadi & Islam, 2020; Li et al., 2021; Nussinovitch, 2010) the methods can be considered based on the applications (Zainal et al.,
where a wide number of materials, including active compounds, phe- 2021).
nolics, drugs, color, flavor, emulsions, probiotics, etc. can be trapped The use of microcrystalline cellulose (MCC) and nanocrystalline cel-
into the gel matrix (Martins, Poncelet, Rodrigues, & Renard, 2017; lulose (NCC) to engineer new products with health well-being is increas-
Saqib, Ahammed, et al., 2022; Simó, Fernández‐Fernández, Vila‐Crespo, ing rapidly due to their superior functionality over other colloids (Nsor-
Ruipérez, & Rodríguez‐Nogales, 2017;Yuan, Yin, et al., 2022). The ver- Atindana et al., 2020; Zhong & Nsor-Atindana, 2021). Since cellulose
satility and diversity of alginate make it the prime choice for hydrogel- itself doesn’t have any gelling properties, it is commonly used as a car-
based systems. It can easily be used in combination with other polysac- rier material with improved mechanical resistance while formulating
charides or proteins where any desired properties can be achieved. The hydrogel beads. The use of MCC and NCC added functionality in beads
monomeric units (M-block & G-block) of alginate can also play a critical prepared with cellulose. The mechanical strength of beads was signifi-
role in designing gel beads (Bennacef, Desobry-Banon, Probst, & Deso- cantly improved for liquid-core or solid beads using different forms of
bry, 2021; Hariyadi & Islam, 2020; Rehm, 2015). cellulose ( Guo et al., 2017; Nie et al., 2021; Svagan et al., 2014).
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Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Table 1
Common food colloids and their properties used to fabricate hydrogel beads.
Colloids name Source Name of binding blocks Applications Pros and cons References
Agar Red algae (Gelidium sp. and It mainly comprises Crushable beads for Thermo-reversible gel, ((Delrieu and Ding, 2001);
Gracilaria sp.) Or seaweeds repeating anaerobioses hydrophobic and widely available, versatile Noreen et al., 2020;
(Sphaerococcus euchema) units alternating between hydrophilic materials, application, poor barrier Sharma, Sharma, & Majumdar,
3-linked entrapment of bacteria, properties, syneresis 2014; Stanley, 2006)
𝛽-d-galactopyranosyl (G) enzyme, used as a laxative,
and 4-linked 3,6- vegetarian
anhydrous-𝛼-l- gelatin substitute in
galactopyranosyl different foods
units
Alginate Brown seaweeds Linear copolymer with Gelation with divalent Most commonly used (Cao, Lu, Mata, Nishinari, &
and few species of bacteria blocks of cations, immobilization material for capsulation, Fang, 2020; Hu, Zheng, Zhao,
(1–4)-linked and encapsulation, appetite poor mechanical and & Yu, 2020; Nordgård &
"-D-mannuronate suppressant, wall material, chemical stability but can Draget, 2021; Saqib, Ahammed,
And L-guluronate a most common material easily be improved in Liu, & Zhong, 2022)
residues, covalently linked for gel bead fabrication combination with other
together in different colloids,
sequences gelation is challenging to
control since the gel
depends on alginate
molecular structure, which
significantly varies upon
species, geography, season
etc.
Cellulose Plant cell wall material and Homo-polymer of " (1, 4) Provide mechanical Insoluble in water, (Ergun, Guo, & Huebner-Keese,
Chemical modification D-glucose stability of beads, an extra inexpensive, some 2016; Ibrahim, Riahi, Said,
layer of protection, chemically modified Sabri, & Rozali, 2019;
encapsulation, filler cellulose has toxicity and Nie et al., 2021;
materials environmental threat Rakhshaei, Namazi,
Hamishehkar, & Rahimi, 2020)
Carrageenan Red seaweeds (Chondrus Sulphated D-galactose and Heat set gel beads, Thermo-reversible gel, (BeMiller, 2019;
Crispus) L-anhydrogalactose desserts, gel to immobilize partial degradation at low Keppeler, Ellis, & Jacquier,
cells/ enzymes pH limits the application 2009; Yermak et al., 2021)
for intestinal or colon
delivery
Guar gum The endosperm of guar A linear chain of Mostly in desserts and Used as a filler or thickener (Eskin, Ikeda, & Cui, 2007;
beans Galactomannan unit yogurt, filler materials of in beads, swelling and Theocharidou, Mourtzinos, &
gel beads obstructing the intestines Ritzoulis, 2022(Lewis, 1992)
and esophagus
Gum Arabic Exudates of A complex mixture of Hard gummy candies, Excellent filler material for
the Acacia tree, (Acacia saccharides and chocolate candies and gel beads, it has some (Sutherland, 2007;Eltayeb, Awad,
Senegal and Acacia seyal) glycoproteins chewing gums minor side effects like Elderbi, & Shadad, 2004)
bloating and nausea (at
high doses); certain
antibiotics and drugs are
reported to interact with
gum arabic
Konjac mannan Tubers of Konjac Glucomannan is Gelling, texturing, and Widely accepted weight (Guo, Yokoyama, Chen, Liu,
(Lasioideae Heteropolysaccharide water binding agent, loss supplement, enhances et al., 2021; )Yang et al.,
Amorphophallus) consisting of provide fat replacement rheological and textural 2017;(Guo, Yokoyama,
D-glucose (G) and properties in fat-free and properties, slows down the Chen and Zhong, 2021)
D-mannose low-fat meat products release of bioactive
(M), linked by " -D-1,4
bonds
With a G/M ratio of 1 to
1.6
Locust bean Extracted from the seeds of Composed of galactose Gelling agent, dispersible Chocolate substitute, lower (Schorsch, Garnier, & Doublier,
gum/Carob gum the and mannose units in either hot or cold water, carbohydrate absorption 1997; Eskin, Ikeda, & Cui,
Carob tree combined Produce gel in the presence 2007;Dakia, Wathelet, &
through glycosidic linkages of sodium borate Paquot, 2007)
described as a
galactomannan
Pectin Hetero polysaccharide Linear Gelling agent, used in Jam, Widely available, cheap, (Cao et al., 2020; Günter &
derived 𝛼-(1–4)-linked jelly, marmalade, non-toxic, pH-responsive Popeyko, 2016; Vityazev et al.,
from the cell wall of a D-galactouronic Jujubes, yogurt, Drug and bio-adhesive. 2020)
higher acid, generally esterified by delivery for colon, Swelling Inconsistent gelling
terrestrial plants, and fruits methyl groups at position control delivery properties and poor
like citrus peel, guava, 6. anionic polysaccharide, Gel beads with reproducibility, high
apple LM-pectin produces gel in combinations of other concentration of sugar or
the presence of Ca and colloids, low pH required for
HM-pectin at low pH, gelling, can be used at a
higher temperature than
other gelling agents
(continued on next page)
4
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Table 1 (continued)
Colloids name Source Name of binding blocks Applications Pros and cons References
Starch Potato, wheat, rice, maize, D-l, 1–4, 1–6 linked Secondary gelling agent, Bacterial adhesion to ( Chen et al., 2021;
Tapioca etc. glucose Cost-effective, used in starch may also provide Lozano-Vazquez et al., 2015;
Polymer, mainly made of combination with other advantages in new Mitchell & Hill, 2021;Anal &
amylose polymers in beads probiotic technologies to Singh, 2007)
(linear) and amylopectin enhance the delivery of
(branched) viable and metabolically
active probiotics to the
intestinal tract
Cheap and does not impart
any taste
Xanthan gum Fermentation of glucose or The polysaccharide chain Emulsion/oil core beads, High shear thinning (Ben Messaoud, Sánchez-
Sucrose by Xanthomonas consists of two viscosifier, help to stabilize behavior, can survive at a González, Probst, & Desobry,
Campestris "-D-glucose” units linked the colloidal oil and solid wide range of pH and 2016; Doublier and
through components against temperatures, one of the Cuvelier, G., 2006; Saqib et al.,
The 1, 4 positions. The side creaming by acting as an widely used thickeners in 2022;
chains emulsifier and texture the food and Sutherland, 2007;Slavin, 2013;
consists of two mannose modifiers in different pharmaceutical industry, Daly, Tomlin, & Read, 1993)
and one foods, core-shell beads over-consuming causes
Glucouronic acid, and thus stomach upset and
the digestive problems, and
the chain consists of can alter gut bacteria
repeating
Modules of five sugar units
Whey Acid or sweet dairy whey, Mainly comprised of Emulsion core beads, Rich in nutrition, it can (Aguilera B., 2004;
Protein separated from the casein globular Gelling agent, and make complexes with other Chen, Yokoyama, Liang, &
curd as the soluble fraction Proteins like thickener in polysaccharides (e.g., Zhong, 2020;Du, Zhou, Lyu,
a byproduct of cheese "-lactoglobulin and the food industry, WP-pectin complex); heat Liu, & Ding, 2022)
production l-lactalbumin emulsifiers in active unstable,pH-sensitive,
emulsion gels environment-sensitive
Chitosan Crustaceans’ shells chitin 𝛽-(1→4)-linked Protein encapsulation The second most abundant (Fernandes, Pereira, do Céu
D-glucosamine Omega-3 rich oil biopolymer, provides an Fidalgo, Gomes, & Ramalhosa,
N-acetyl-glucosamine encapsulation Coating extra layer of protection 2020; Hamed et al., 2020;
capsules, gel beads texture for beads or film, improves Kulig, Zimoch-Korzycka,
and mechanical resistance barrier and mechanical Jarmoluk, & Marycz, 2016;
properties, only solubility Romo, Abugoch, & Tapia,
in acid limits some 2020;
application, can interfere (Qu & Luo, 2020)
with fat-soluble vitamins,
sensitive to allergic people,
and has a negative
interaction with a few
drugs
Gelatin Animal skin and bones Protein high in glycine and Filler in gel beads in Water-soluble, (Courts, 1977; Oakenfull, 1987;
(made Proline combination with other heat-sensitive, can change Schrieber & Herbert, 2007;
By partial hydrolysis of polymers, material properties Zeeb, Saberi, Weiss, &
Collagen of animal Gelling agent in gelatin (elasticity, stiffness, tensile McClements, 2015)
Connective tissue) desserts, strength) without affecting
Yogurt, cream cheese and the microstructure
Margarine
Soya proteins Soybeans Interaction of two globulin Heat set gel, prepare food An inexpensive source of (Bhattacharya & Jena, 2007;
Proteins like glycinin and emulsions, emulsion beads protein, inferior Lin, Kelly, Maidannyk, & Miao,
"-conglycinin mechanical properties, 2020)
high moisture sensitivity
Zein Corn Peptide chain containing Zein nanoparticles, surface High resistance to heat, (Liu, Fishman, Hicks, Kende, &
Mainly prolamine coating, microbeads, water, and good oxygen Ruthel, 2006; Tortorella et al.,
Pickering emulsion, barrier properties, coating 2021; Yuan, Ma, Xu, & Wang,
stabilizer, smart carrier for foods and drugs, 2022; Zhang et al.,
Delaying the release of alternative for synthetic 2022;Tortorella et al., 2021)
color and flavor from gel polymer, improved control
beads release properties,
Water-insoluble, foul odor
and color
Apart from that, they also can contribute to the stability and reten- Liu, Li, Cheng, & Liu, 2019). They are an effective carrier for bioac-
tion of beads. Even though they may not be the most important part tive compounds, fats, oils, fatty acids, and flavors (Lingyun Chen et al.,
of the structure, the contribution of these food colloids is noteworthy, 2006; Jia, Dumont, & Orsat, 2016). The most common animal pro-
and more and more applications are under investigation. teins used in encapsulation are whey protein, casein, gelatin, and col-
lagen, while plant-derived proteins are soy protein, zein, and gliadin
3.2. Protein-based materials (Tarhini, Greige-Gerges, & Elaissari, 2017).
Proteins are generally regarded as safe (GRAS) and have high nu- 3.2.1. Whey protein
tritional significance. They are insoluble in acidic conditions and eas- Whey proteins have a higher degree of compatibility in gelling and
ily dissolved at alkaline pH Chen, Remondetto, & Subirade, 2006; emulsification. Lactoglobulin and lactalbumin are the most common
5
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
whey proteins suitable for encapsulation purposes. Several recent stud- 4. Types of gel beads
ies also showed that whey proteins help encapsulate bioactive com-
pounds, either on their own or with the help of other carrier compounds Gel beads can be classified based on their structure, properties, and
(Devi, Sarmah, Khatun, & Maji, 2017; Bilek, Yılmaz, & Özkan, 2017; applications. Nano, Micro, Macro, and milliliter sizes are all possible.
Faridi Esfanjani, Jafari, & Assadpour, 2017). Beads can be divided into the following categories based on their struc-
ture. Depending on the intended use, these types may be of various sizes.
3.2.2. Gelatin • Solid gel beads: These are the most common and popular kinds of
Gelatins obtained from animal collagen protein can be of two types
beads. These beads can easily be manufactured from a variety of
depending on whether they’ve gone through partial hydrolysis by acid or
materials. It can be made from a single material or a combination
alkaline. Gelatin A is obtained from fish skin, porcine or bovine through
of different colloidal materials. A wide range of active ingredients
acid hydrolysis. Gelatin B is obtained from the earlier sources through al-
has been reported to be trapped inside solid gel beads. Colloidal ma-
kaline hydrolysis (Ninan, Jose, & Abubacker, 2011). Gelatins have good
terials act as a retarding matrix in hydrogel beads. The active com-
functional characteristics in terms of biocompatibility, biodegradability,
ponent may or may not interact with the gel matrix. Table 2 shows
water retention ability, film formation ability, and anti-carcinogenicity;
some examples of these types of beads.
therefore, they are suitable materials for encapsulation (Ahammed, Liu, • Liquid-core gel beads: This type of bead has an aqueous core cov-
Khin, Yokoyama, & Zhong, 2020; Deng, Kang, Liu, Feng, & Zhang,
ered by a seamless shell or membrane and is often referred to as
2017).
a reservoir system. The membrane can function as a barrier or as
a control for diffusion. This type of bead is generally produced by
3.2.3. Collagen the ionotropic gelation method. A liquid droplet can be shaped into
Collagen is a hierarchical coating material with excellent tensile an insoluble cavity by a controlled ionic interaction between an an-
properties derived from the skins and cartilage of animals. The high ionic and cationic polymer within the boundary condition. These
mechanical strength of the fibers, low antigenicity, suitability as a beads have recently gained popularity as directly edible beads with
substrate for cell growth, and tunable stability by chemical or phys- an exciting bursting mouthfeel (Bremond, Santanach-Carreras, Chu,
ical crosslinking are some of the outstanding properties of collagen & Bibette, 2010; Saqib, Ahammed, et al., 2022).
(Radhakrishnan, Nagarajan, Bechelany, & Kalkura, 2020). Collagens are • Emulsion core gel beads: This is comparable to the liquid-core
extensively used in a colloidal system combining with other proteins or beads mentioned above, with the exception that the core material
polysaccharides. could be an emulsion, nanoemulsion, liposome, or emulsion gel.
This type of bead is commonly used with hydrophobic materials.
3.3. Selecting the appropriate material for beads Since the demand for functional foods is growing, food manufac-
turers and researchers are increasingly interested in developing hy-
Edible hydrogel beads for food applications are demanding. Proteins drophobic delivery materials. Numerous scientific papers describe
and polysaccharides are two of the main sources for making beads. How the encapsulation of versatile, functional components in emulsion
edible hydrogel beads are used and how well they work in food systems beads and their successful delivery to the target site with high effi-
depend heavily on their properties. Besides, dealing with food appli- ciency (Feng, Yue, Wusigale, Ni, & Liang, 2018; Lin, Kelly, & Miao,
cations is more challenging since sensory, safety, shelf life, consumer 2020).
• Double encapsulated beads: Compared to the other types of beads,
acceptance, and price must all be considered. Regardless, all of the
above-mentioned materials are from natural sources, they have flaws on this one is quite intriguing and intricate. This may also be de-
one side or the other. Alginate, chitosan, pectin or Gellan gum is ionic scribed as the combination of beads described previously. In this
polymers, and they can undergo ionotropic gelation, while agar, car- type of bead, microbeads are typically re-encapsulated within rela-
rageenan, gelatin and some proteins are thermos-reversible gel. There- tively larger beads. In one system, two materials with opposing or
fore, combining two or more polymers is becoming trending. For exam- incompatible properties can be encapsulated. Probiotics and antibi-
ple, alginate has poor mechanical properties, but alginate-chitosan or otics, for example, were encapsulated in an alginate matrix ( Li et al.,
alginate-cellulose beads showed improved stability (Qu & Luo, 2020). 2018).
Similarly, whey protein is very sensitive to the environment, but whey
protein-pectin conjugate produces stable beads (Du, Zhou, Lyu, Liu, & 5. Production techniques
Ding, 2022). Other polysaccharides, such as xanthan gum, guar gum,
locust bean gum, and others, which are commonly employed as thicken- Gel beads are currently being made for texture modification, encap-
ers or filler materials in gel beads, have their individual acceptability. A sulation, and targeted delivery. The method of production must be cost-
targeted delivery site is another important consideration while choosing effective, versatile, reproducible, and relatively straightforward. Vari-
material. For example, agar beads can be suitable for oral delivery, but ous techniques have been used to encapsulate bioactive compounds on
transport up to the colon requires materials that can survive the harsh beads, considering the nature of the finished beads, their intended use,
gastric environment (e.g., konjac) (Ma, Peng, Tang, & Cheng, 2021). the nature of the core material, their release site, particle size, and so
Textural and sensory qualities are also essential. Objectionable flavor, on. The methods are chosen according to a precise objective, taking into
color, taste or mouthfeel restricts their applicability in food. account the effectiveness of the encapsulation, the rate of production,
Nevertheless, the choice of material is totally dependent on the and the adequacy of the process (Jafari, Assadpoor, Bhandari, & He,
specific use and design of beads. In recent studies, alginate-based gel 2008). For different types of beads to entrap hydrophilic, lipophilic, and
beads have received significant attention for their ability to undergo hydrophobic materials, many methods have been introduced, including
ionotropic gelation. Innovations in fabrication processes are also emerg- various types of extrusion, spray, spinning, and many more (Ching et al.,
ing, with more and more techniques such as particle/fiber-reinforced 2017). While fabricating gel beads with an active group, it is critical to
hydrogels, double networks, dual cross-linking, freeze-thaw cycles, and think about how the encapsulant will be immobilized. Therefore, the
physical conditioning demonstrating superiority to conventional meth- methods are described in two categories below, and the most commonly
ods (Khalesi, Lu, Nishinari, & Fang, 2020). Some advantages and disad- used techniques are discussed.
vantages and applications of these materials are compared in Table 1.
These biopolymers have the potential to create and modify the structure, 1 Methods for fabricating hydrogel beads (e.g., extrusion, spray dry-
texture, sensory properties and shelf life of food products. ing, etc.)
6
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Table 2
Hydrogel beads fabricated with functional groups.
Tea polyphenols Alginate, Inulin, Gam Arabic, Chitosan Composite solid gel beads (Li et al., 2021)
Curcumin Alginate Emulsion filled alginate beads (Song, Wang, Qian, Zhang, & Luo, 2012;
Zeeb et al., 2015)
Plant polyphenols (leaf extract) Alginate Liquid-core alginate beads (Tsai, Kitamura, & Kokawa, 2017)
Plant extract (vegetable Alginate Ca–alginate microbeads (Aguirre-Calvo, Aguirre-Calvo, Perullini, &
byproduct) Santagapita, 2021)
Plant extract (medicinal herb) Alginate, Inulin Ca–alginate microbeads (Balanč et al., 2016)
Plant extract (aromatic herbs) Alginate Ca–alginate microbeads (Tomé & da Silva, 2022)
Chlorogenic acid Alginate, Tapioca Starch Alginate macro beads (Lozano-Vazquez et al., 2015)
𝛽-carotene Alginate Ca–alginate microbeads loaded with Nano ( Zhang, Zhang, & McClements, 2016)
emulsion
Enzyme Agar Agar hydrogel beads (Sharma et al., 2014)
Oil Alginate, Shellac Alginate-shellac wall material, (Martins, Poncelet, Rodrigues, & Renard,
Alginate as matrix 2017; Morales et al., 2017)
Omega-3 Sodium caseinate, alginate Nano emulsion loaded micro-beads (Chen et al., 2017)
Bovine serum albumin (BSA) Cellulose (Micro Crystalline Cellulose) Microbeads (Nie et al., 2021;
Alginate Ca–alginate gel beads (Hu, Zheng, Zhao and Yu, 2020)
Drug (allopurinol) Gelatin Oral dissolving beads (Murata, Isobe, Kofuji, Mizutani, &
Kamaguchi, 2012)
Antibiotic (Ciprofloxacin) Chitosan, Alginate Chitosan coated alginate beads (Kyzioł, Mazgała, Michna, Regiel-Futyra, &
Sebastian, 2017)
Antibiotic (Amoxicillin) Carboxy methyl cellulose Bio-nanocomposite hydrogel beads (Behzadi Nia, Pooresmaeil, & Namazi, 2020)
Caffeine Alginate, Pectin, Carrageenan, Chitosan, and Composite millimeter-sized beads (Belščak-Cvitanović et al., 2015)
Psyllium
Enzyme (Protease) Pectin, Resistant Starch Hybrid pectin starch microbeads (Mala & Anal, 2021)
Enzyme (lactase) 𝜅-Carrageenan Enzyme loaded solid beads ( Zhang, Zhang, Chen, & McClements, 2016)
Probiotics Whey Protein (WPI), Shellac Spray-dried microcapsules (Yin et al., 2022)
Probiotics Sodium Carboxymethyl Cellulose (CMC), pH-sensitive hydrogel beads (Wang et al., 2021)
Chitosan, Alginate
Ibuprofen Gelatin Soft chewable beads (Hattrem, Dille, Seternes, Ege, & Draget,
2018)
Resveratrol, 𝛼-tocopherol WPI, Alginate Emulsion filled gel beads (Feng, Yue, Wusigale, Ni, & Liang, 2018)
Vitamin B12 and Vitamin C Alginate, Chitosan Spray-dried microbeads (Estevinho, Carlan, Blaga, & Rocha, 2016)
2 Methods for incorporating bioactive within beads (e.g., emulsifica- korb, 2019; Hariyadi & Islam, 2020; Larosa et al., 2018; Lupo, Maestro,
tion, coacervation, liposomes etc.). Gutiérrez, & González, 2015; Martins, Renard, Adiwijaya, Karaoglan, &
Poncelet, 2017; Saifullah et al., 2019).
5.1. Extrusion Although extrusion by syringe is the simplest method of produc-
ing uniform gel particles, this method produces large gel particle sizes,
The most common and widely used approach for producing gel beads and scale-up difficulties limit this method to a lab-scale setup only. In
is simple dripping or extrusion (Davarcı, Turan, Ozcelik, & Poncelet, addition, this method is also limited to solution with a low viscosity
2017; Kuo & Ma, 2001; Li, Hou, Li, Zheng, & Li, 2013; Lim, Lee, Ah- (<200cP) due to pumping difficulties and needle blockage (Prüsse et al.,
mad, Singh, & Ravindra, 2016; Puguan et al., 2014). Extrusion is a gen- 2008). The large particle size also requires freshly made particles to
tle and convenient method that can successfully encapsulate a variety be cured in the gelling bath for a period of time. The droplet surface
of compounds, including hydrophilic or hydrophobic compounds with gels instantaneously upon entering the gelling solution. A longer time
a long shelf life (Jia et al., 2016). In general, beads greater than 1.0 is needed for the cations to diffuse into the interior of the droplet, de-
mm in diameter can be prepared by using a syringe with a needle or a pending on gel particle size. However, the extrusion technique produces
pipette (Gray & Dowsett, 1988; Traffano-Schiffo, Castro-Giraldez, Fito, relatively large particles with a porous structure, limiting its industrial
& Santagapita, 2017; Wee, S., Gombotz, 1998). A dripping solution that application for controlled release and high stability. But this is advanta-
may or may not contain active compounds is transferred drop-wise into geous for large spherical beads, especially where the inotropic gelation
a gently agitated gelling solution. The basis of this method involves the technique is used for masking biomaterials. However, extrusion drip-
drop-wise extrusion of charged polymer droplets from a loaded syringe ping with different mechanical setups can produce beads with a wide
into an opposite charge gelling bath. For example, alginate beads pro- range of particle sizes (from nano to micro).
duced by simple dripping are generally in the millimeter size range (1– An alternative to the normal dripping encapsulation is reverse gela-
2 mm) ( Chan et al., 2011; . Li et al., 2013). Examples of compounds tion/spherification. Fabrication of liquid core beads through reverse ex-
encapsulated with this method include cells, oils, enzymes, flavors, and trusion dripping has been utilized by several research groups (Saqib, Liu,
plant extracts (Déat-Lainé, Hoffart, Cardot, Subirade, & Beyssac, 2012; et al., 2022; Tsai, Kitamura, & Kokawa, 2017). This method facili-
G. Gómez-Mascaraque, Martínez-Sanz, Hogan, López-Rubio, & Brod- tates the advantage of incorporating versatile ingredients, greater gel
7
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Fig. 1. Different methods for producing beads. (A) Techniques for fabricating gel beads (B) Techniques for incorporating bioactives in beads. The figure of liposome
was adapted from (Ioele, De Luca, Garofalo, & Ragno, 2017) with permision.
strength, higher stiffness, less thickness, smooth surface, and better per- the dryer. Bakry et al. (2016) reported that hydrophilic polysaccharides
meability ( Chan, Lee, & Heng, 2006). The extrusion technique can be fa- (e.g., maltodextrins, chitosan, alginate, and different gums) and proteins
cilitated and equipped in many ways, i.e., application of a multi-nozzle- are predominantly used as carrier agents, and active hydrophobic or hy-
system or rotating disk, centrifugal extrusion, co-extrusion, electrostatic drophilic compounds are the core material in spray drying. Spray drying
extrusion, and melt extrusion (Lević et al., 2014; Rodríguez, Martín, optimization and modification are also quite prevalent, with numerous
Ruiz, & Clares, 2016). A brief description of different extrusion drip- parameters considered for reliable end goods.
ping is illustrated in Fig. 1 (A). Despite the fact that the physical and For instance, for encapsulating food flavor compounds, spray chill-
mechanical properties of gel beads are completely dependent upon a ing/cooling is the most promising and emerging strategy. It sets the at-
number of inconsistent factors like intrinsic properties of biomaterial omized fluid beads into particles from a couple of microns to millime-
or processing conditions, some research groups have optimized a few ters. Lopes et al. alluded to this encapsulation method as spray cooling,
mathematical models for predicting gel beads’ properties produced by spray congealing, or prilling. de Souza Simões et al. (2017) found sim-
extrusion dripping (Bennacef, Desobry-Banon, Linder, et al., 2021; E. S. ilarities between spray chilling and spray drying principles, including
Chan, Lee, Ravindra, & Poncelet, 2009; Kim, Jeong, Cho, & Kim, 2019). atomization, particle development, and particle collection. It is a low-
cost, efficient method for the entrapment of compounds. But this method
5.2. Spray drying is not suitable for thermosensitive materials like probiotics.
8
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
There are four simple steps to freeze-drying: freezing, primary dry- carotene (Jain, Thakur, Ghoshal, Katare, & Shivhare, 2016), and antho-
ing, secondary drying, and final treatment (Abdul‐Fattah, Kalonia, & cyanins (Arroyo-Maya & McClements, 2015). Combination of nisin and
Pikal, 2007). Freeze drying could be beneficial in two aspects. Firstly, avocado antioxidant extracts (Calderón-Oliver, Pedroza-Islas, Escalona-
the entire drying method is administered under vacuum conditions; Buendía, Pedraza-Chaverri, & Ponce-Alquicira, 2017) and bioactive
thus, there’s a sensible absence of air that doesn’t enable aerophilic compounds from broccoli (Sánchez, García, Calvo, Bernalte, & González-
degradation. Secondly, the drying temperature is not up to the ambi- Gómez, 2016).
ent temperature. Compounds that are very susceptible to oxidation and However, the production cost of the agglomeration method is high,
thermal degradation (such as fragrances) can be dried in a vacuum with depends on many factors (such as pH value and ionic strength), has lim-
minimal physical and chemical damage. ited stability in various aqueous solutions, and it is not easy to strictly
Recent studies have conjointly been reportable on pepper natural control particle size and prevent particle aggregation (Jia et al., 2016;
resin spicy flavor, caffeine, and peppermint oil (Chen & Zhong, 2015; Joye & McClements, 2014) Optimizing coacervation conditions is criti-
De Aguiar, Silva, Alves De Rezende, Barbero, & Martínez, 2016; cal to successfully applying complex coacervation because the stability
Fuciños et al., 2017). However, higher energy requirements and pro- of coacervation complexions is limited by the narrow range of pH, ionic
longed duration (at least 20 h) are the most important disadvantages of strength, and temperature. In addition, the optimal conditions for the
freeze-drying (de Souza Simões et al., 2017). In addition, freeze-drying coacervation process need to change depending on the coating and cop-
will produce irregularly shaped open porous structures, which are inef- ulating material (Timilsena, Wang, Adhikari, & Adhikari, 2017).
fective when the sustained release of flavoring compounds is required
(Hundre, Karthik, & Anandharamakrishnan, 2015). 5.6. Liposome
9
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
food science, such as building foods with the required exciting texture, The changes in properties due to crosslinking are crucial and ad-
maintaining metastable food structure and extending shelf life, design- vantageous while designing beads for a particular purpose. A hydro-
ing food packaging, nutrition, delivery and bioavailability, calorie con- gel polymer can be synthetic or natural, formed by homopolymers or
trol, and food safety monitoring. co-polymers. Hydrogels can form three-dimensional netlike imperfect
It is tough to predict the long run of gel science accurately, and it macromolecular network structures by linking multiple chains at spe-
is also challenging to accurately predict the application potential of hy- cific binding sites (Fig. 3 (A). Thus, huge amounts of water are trapped in
drogels in food science. Both colloidal gel science and food science are the gel network by hydrogen bonds. Polysaccharides, proteins, or inter-
developing rapidly. The current review discusses the application method operating these two are the most common types of hydrogels that have
of hydrogel beads in food science. Hydrogels are good candidates for use been utilized so far. There are two approaches to making crosslinked
in delivery systems because they can take in and hold a large amount hydrogels.
of water or biological fluids in a 3D network shape ( Liu, Huang, Chen,
1 Chemical crosslinking.
Lin, & Wang, 2019; McClements, 2017).
2 Physical crosslinking.
Other properties of hydrogel beads, such as response to stimuli to
heat, pH, and light, are beneficial for controlled release into food de- In chemical crosslinking, generally, a crosslinker (e.g., glutaralde-
livery systems (Cooper & Yang, 2019). Hydrogel beads can also play an hyde, transglutaminase, formaldehyde, dialdehyde) is used to form a co-
essential role in reducing calorie intake, improving satiety, or reducing valent bond (Ahammed et al., 2021; Maitra & Shukla, 2014; Zhu, 2010)
intake (Cao & Mezzenga, 2020).Wu et al. (2014) created hydrogel gran- (Fig. 3 (B)). Chemically crosslinked gels are mechanically strong and
ules from protein and fiber in fine soft substances that can be a healthier chemically stable, but for food applications, sometimes these crosslink-
replacement for starch granules. Thompson et al. (2017) reported using ers are associated with health hazards. Physical crosslinking does not
a temperature-insensitive food-grade methylcellulose hydrogel blend to require any chemical agent to form a gel. Generally, these are ionically
reduce the heat density of pancakes cooked at temperatures well above crosslinked, and there is weak interaction between polymer chains, for
the boiling point of water. Chung et al. (2013) reported that emulsion example, sodium alginate. Physical crosslinking is inhomogeneous and
hydrogels in food products reduce the fat content by replacing animal free chain ends or chain loops are available in the gel network. So, these
oils with vegetable oils. gels are not permanent and often reversible (Wang et al., 2019). The
The hydrogel beads have important structural properties (elastic- properties of physically crosslinked gels are largely dependent on tem-
ity, stiffness, impact strength, and fracture toughness) as soft materials. perature, material properties, monomeric compositions, pH, concentra-
Therefore, in addition to being used as a replacement to reduce calories, tion, etc. Physical and chemical crosslinking are often used in tandem.
hydrogels can also improve texture or mouthfeel. For example, emulsion Physically formed protein-based gels, for example, can be chemically
hydrogels can affect the textural properties of foods (Dickinson, 2012). crosslinked to improve their mechanical properties.
Interestingly, replacing meat or starch with hydrogels with excellent Thermal gelation, or heat-induced gelation, is another very common
textural characteristics or low oil content is also an effective way to re- and significant process of gelation. The molecules unfold or dissociate
duce the calorie content of foods. Because the hydrogel has a high-water due to the absorption of energy produced by heat, then aggregate by the
retention capacity in its structure, the three-dimensional hydrophilic association of helices. After cooling down, they become rigid. For exam-
polymer network can allow many molecules or ions to diffuse through ple, the gelling process of carrageenan has been illustrated in Fig. 3 (C).
the system freely. The aggregation of helices produced stable gels, and the presence of
In addition, the high adsorbent with high porosity, large surface salt increased the aggregation. In some cases, just heating will cause
area, and reusability makes the hydrogel beads an effective platform co-polymerization (Redaelli et al., 2017).
for adsorption or removal activity (Gonçalves et al., 2017, 2018; Crosslinked polymer chains bring about significant changes in phys-
Guo et al., 2019; He et al., 2020; Wang et al., 2019). For example, ical and chemical properties depending on crosslinking degree, crys-
Gonçalves et al. (2020) developed a promising adsorbent based on chi- tallinity, crosslinkers, and polymer properties. Among the changes: de-
tosan hydrogel beads substrates modified with carbon nanotubes to re- crease or increase of elasticity, decrease in flow behavior, Increase in
move food dyes in simple, binary aqueous systems. polymer strength and toughness, Increase in hydrophobicity, changes
In addition, there are many research in the environmental sciences in glass transition temperature change to thermoset from thermoplastic
on using hydrogels to remove heavy metals and other contaminants that are most notable where most of the properties are irreversible (Maitra &
could also be considered for applications in food science. Shukla,2014). Crosslinking is a fundamental process for the production
of hydrogel beads. So far, it has been the most widely utilized approach.
A regulated gelling technique is a must to develop the desired attributes
7. Gelling mechanism of hydrogels of the final beads. Ionotropic gelation of sodium alginate or heat set
gelation of agar or carrageenan can be mentioned as an example in this
In polymer chemistry, crosslinking is a stabilization process whereby regard.
polymer chains are linked with each other by an ionic or covalent bond.
Crosslinking restricts the mobility of polymer chains, transforming a liq- 8. Release of active materials from beads
uid state into a solid or gel state. As a result, the individual properties of
free-moving polymer chains are altered. Crosslinking enhances the me- Hydrogel beads have proven to be a versatile tool for preserving and
chanical, chemical, and thermal properties of any polymer. On the other transporting a wide range of functional components. Fabricating beads
hand, hydrogels are polymer structures that can contain a large amount for the food sector is more challenging and sophisticated due to concerns
of water or biological fluid. So, applications in food science, especially about safety, taste, and consumer impression. However, one of the key
as beads, crosslinked hydrogels are widely utilized as carriers or shell concerns for edible hydrogel beads is the stability and controlled release
materials for the delivery of functional materials. of active ingredients at a particular site. Table 2 outlines some recent
The water status in a hydrogel is another important consideration. improvements in the application of hydrogel beads using various bio-
Water accommodated in a gel network can be classified into four groups, materials and functional groups.
such as free water, interstitial water, bound water, and moderately
bound or semi-bound water (Redaelli et al., 2017). The final gel proper- 8.1. Release mechanisms
ties (mechanical, physical, or release properties), stability, and perfor-
mance largely depend on the amount and type of water. Different types Materials are basically diffused from hydrogel beads by the following
of water in a hydrogel are illustrated in Fig. 2. mechanisms. These mechanisms are illustrated in Fig. 4.
10
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Fig. 3. Different Gelling mechanisms for food colloids: A: ionic (physical) crosslinking (example Sodium alginate) B: Chemical crosslinking (example Gelatin-Zein
crosslinked by Transglutaminase) C: Temperature set gels (example: 𝜅-carrageenan; : K+ ion) D: Temperature set gel (example: Gelatin).
11
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
sically by diffusion. If in the diffusion-controlled system, the matrix or 8.2. Mathematical models for predicting solute release from gel beads
coating is unaffected by the surrounding liquid, the matrix is thermody-
namically triggered by changing its glassy state, and active agents come It is necessary to understand and evaluate the release properties for
into contact with the penetrant. The diffusion or release kinetics are al- effective design and delivery of gel beads. Many mathematical models
most similar to diffusion-controlled release; just need to consider the have already been developed and validated (Bruschi, 2015). Mathemat-
swelling zone and swelling rate of a particular biomaterial. Sometime ical models are developed to describ release of materials as a function of
dehydrated rigid polymer states are also used to carry active agents that time. These models are very useful for predicting the release mechanism
are later utilized by swelling-controlled diffusion. In a porous or microp- in a gel bead system. The kinetic models depend on transport mecha-
orous membrane or matrix system, the pore size increases after swelling, nisms, dissolution behavior of the gel matrix, surrounding medium, etc.
and core materials diffuse out. One gel bead system may have different release properties in different
Shrinking: This is the opposite of the swelling controlled system. mediums. Therefore, the actual diffusion is more complex and difficult
Active materials are loaded in a swelling state and released by shrink- to predict. So, many models have been developed considering differ-
ing. For liquid core beads, due to osmotic imbalance or pressure, core ent factors. For example, Eq. 1 is developed for simple diffusion from
materials diffuse into carrying active materials, and the volume of beads the matrix system, and Eq. 2 is for release from heterogenous erosion
shrink. (Pothakamury & Barbosa-Cánovas, 1995). The basic release properties
Fragmentation: This is the physical disruption of the carriers. The are described by zero-order and first-order reaction kinetics. Some com-
matrix is fragmented by shear or compression force and active materials monly used kinetics model are tabulated in Table 3.
are released. For liquid core beads, this phenomenon is often termed [ ]
𝑀𝑡 ∑∞
8 −𝐷𝑚 (2𝑛 + 1)2 𝜋 2 𝑡
bursting. This happens basically in the mouth or in the digestion process. =1− 𝑒𝑥𝑝 (1)
𝑀∞ 𝑛=0 (2𝑛 + 1) 𝜋
2 2 𝛿2
This release process is very fast.
Erosion: In this process, the active agent’s carrier undergoes deteri- Where
oration by physical, chemical, or enzymatic processes and releases ma- M∞ is the amount of active materials at a finite time
terials. This process can be homogenous or heterogeneous. It may erode Dm is diffusion co-efficient
from surface to core gradually or can erode totally. In the latter pro- 𝛿 thickness
𝑀𝑡
cess, the external fluid enters the bulk matrix by breaking bonds and
𝑀
is <0.6 at early stage and >0.6 and <1.0 later stage
∞
transporting the trapped materials into the surrounding liquid system.
The erosion rate depended on the physicochemical stability of the ma-
[ ]
trix, the molecular weight or gelling mechanism of biopolymers, or the 𝑀𝑡 𝑘 𝑡 𝑛
=1− 1− 0 (2)
efficacy of the release medium. 𝑀∞ 𝐶0 𝑅
There are different types of release that can be controlled
for controlled transport through beads (Pothakamury & Barbosa- 𝑘0 , erosion rate constant
Cánovas, 1995). Such as: C0 , Initial concentration
M∞ , Total amount of active ingredient
• Diffusion controlled release
• Barrier controlled release 9. Designing hydrogel beads for active delivery
• Pressure controlled release
• Solvent activated release Before designing a hydrogel-beads-based delivery system, the pre-
• Osmotically controlled release requisite question will be why do we need to use a functionalized deliv-
• pH-controlled release ery system for foods? There are many food components that cannot be
• Temperature controlled release used simply in foods in their regular form (e.g., some essential lipids,
• Melting controlled release vitamins, flavors, antimicrobials, etc.). A special delivery system is re-
• Combination of two or more systems quired to successfully incorporate them into the food matrix where they
12
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
Table 3
Commonly used diffusion models to describe releases from hydrogel beads—adapted and modified form (Fathi, Donsi, & McClements, 2018) with permission.
can withstand the adverse effects of physical–chemical degradation. An- • Structure and dimension: Hydrogel beads are generally spherical
other reason is that some active compounds need to be delivered to a in shape. But other shapes, like pears, cylindrical, or irregular shapes,
particular site of action. To transport these components up to the tar- can also be formed (Cao & Mezzenga, 2020). Depending on the in-
get site while protecting them from a hostile environment, carrier or dented use, the beads can range in size from micrometers to several
coating materials are used. Among other uses, improving handling and millimeters. Direct edible gel beads specially designed for the es-
storage, masking off-flavor, extending product shelf life, and enhancing thetic purpose or texture modifier shape are very important. But a
foods’ sensory attributes can be mentioned. So, it is clearly delineated carrier with other systems in a matrix shape may affect release and
that the design of hydrogel beads will be extremely divergent and per- stability since they can hardly be seen by the naked eye.
tinent to the specific intention. For example, protein is digested in the • Gels bead Biocompatibility: The biocompatibility and bioavailabil-
stomach while fiber is indigestible and can resist degradation up to the ity of gel beads during transport and dissolution are very complex
colon. Therefore, in designing a delivery system for any particular loca- and significant. Hundreds of factors may be involved in the human
tion of the human GI tract, an in-depth understanding of the mechanisms digestion track. Based on gel bead formulations, the GI environment
and interactions of the carrier matrix and active materials is a prereq- can be influenced by ionic strength, pH, surface charge, electric po-
uisite. At the same time, it is also necessary to make sure the active tentials, enzymes, flow behaviors, internal forces, binding to the bi-
component remains uninterrupted or does not produce any undesired ological surface, etc (Kharkar, Kiick, & Kloxin, 2013; Redaelli et al.,
secondary component throughout the whole process. For example, milk 2017).
protein was reported to interact with some polyphenolic compounds • Gel bead stability: The fabricated gel beads must be stable up to the
(Serafini, Ghiselli, & Ferro-Luzzi, 1996) and some bioactive peptides, target site of action unless every triumph will be meaningless. The
and was encapsulated to mask their undesirable bitter taste (Sun, Ok- active site may be anywhere from the mouth to the colon (Đorđević
agu, & Udenigwe, 2021). A hydrogel bead may not always be designed et al., 2014). For example, if a bead is designed for a textural pro-
only to be transported through the GI tract. It can also be fabricated to file, it must uphold its texture during oral processing from storage,
increase a food’s shelf life, esthetic value or sensory value. freezing, or osmotic environment; if it is designed for the colon, it
In order to develop hydrogel beads for active delivery following at- must survive from oral processing, gastric environment, or intestinal
tributes may need to consider (McClements, 2012). digestion (Shahidi, Ambigaipalan, Abad, & Pegg, 2020).
• Food grade
•
11. Challenges and future trends
Economic production
• Food matrix compatibility
•
There has been a significant amount of research on active delivery us-
Protection against chemical degradation
•
ing biomaterials, and currently, many encapsulation technologies have
Loading capacity and retention:
•
already been introduced in pharmaceuticals, cosmetics, and health care
Delivery mechanism
•
products, but the food industries are still lagging behind. There are very
Bioavailability/bioactivity
limited and classified hydrogel-based food products currently available
on the market. The main challenge for the food industry is to make sure
10. Fundamental considerations for fabricating beads (with the ingredients and delivery system are food grade and relatively inex-
selective attributes) pensive. People won’t buy food with the same money they are ready to
spend on cosmetics, medicine, or health care products. Thus, the fab-
• Gel bead composition: The most preeminent parameter that needs rication methods for hydrogel beads must be in accordance with food
to be considered before designing hydrogel beads is the gel beads’ safety, economical, robust, and reproducible. The taste and smell of the
composition. How a delivery system reacts, how efficiently it will de- food itself is still a major challenge for active delivery via food. It will
liver, how the intermediate reactants will react, the active compound not matter how efficient, effective, or essential a compound it is, unless
and delivery matrix stability and sensitivity, how the matrix disasso- the food becomes attractive and tasty. Consumers’ perception of food is
ciates and reacts in different triggering conditions (e.g., temperature, very complex and personalized. In our present food system, foods still
pH, enzyme); these are all the essential properties (Augustin & San- remain common for all people. But personalized food production is in
guansri, 2012). Along with these regulatory and safety concerns, en- demand, and industries are focusing on that. Personalized foods mean
vironmental issues, labeling, certification, or a special requirement foods that meet a specific person’s demands or choices. We can only find
like halal, kosher, or vegetarian needed to be addressed. infant or baby foods while there is little or no work for elderly people.
• Release mechanisms: Gel beads may have many different re- But elderly people require special attention in terms of food choice as
lease profiles depending on the specific purpose, such as burst their digestive systems change with age. Again, any specific group of
release, sustained release, triggered release, and targeted release people may have food sensitivity (for example, food allergen) or special
(McClements, 2012). needs (for example, specific vitamin-rich food). We eat food for basi-
13
Md.N. Saqib, B.M. Khaled, F. Liu et al. Food Hydrocolloids for Health 2 (2022) 100073
cally two reasons. There is a difference between food preferences and research endeavors are being initiated to achieve high sensory percep-
demand among countries. The first is to satisfy our hunger, and the sec- tions of gel beads. Beads have already become a part of many frozen
ond is to meet our nutritional and sensory requirements (Mackie, 2012). desserts and drinks. This indicates the potential and prospect of hydro-
In the least developed and developing countries, people can hardly meet gel beads in the future. But currently, there are many limitations hin-
their nutritional demands while striving for a full-filled stomach, while dering the application of gel beads that need to be overcome. However,
in developed countries, the sensory and functional attributes are very developing a sustainable gel bead-based food system requires a trans-
demanding, and people are suffering from obesity due to overeating. disciplinary and multi-disciplinary approach, including food scientists,
Therefore, a country-specific demand also needed to be addressed. For- technologists, industrial chemists and engineers, doctors, and dietitians.
mulation of hydrogel-based foods with bioactive compounds (e.g., hy- The relentless pursuit of the goal is to develop edible gel beads with ver-
drogel beads) is a promising solution to meet the highly personalized satile, controllable features, mechanical stability, and exciting texture
and country-wise demand for food in the near future. with a wide range of sensory perceptions and, most importantly, human
Now the research trend is moving towards developing new food- contentment.
grade biomaterials and emerging processes with more efficiency, keep-
ing in mind current limitations. For example, some protein-based hy- Ethical statement
drogel systems can be allergic or sensitive to a certain group of people.
Furthermore, modified proteins or starch may have less consumer ap- This study does not contain any human or animal study.
peal due to a lack of natural labeling. Sensory perception of biomateri-
als is still not widely popular. Scientists are considering all these issues Conflict of interest
and trying to develop cost-effective bio-materials since cost and taste
are among the major challenges for developing a hydrogel-based active The authors declare no conflict of interest.
delivery system. With the evolution of the concept of molecular gastron-
omy, liquid core or acquis core hydrogel beads have attracted significant Acknowledgments
attention from consumers as they have exciting explodable textures. The
size of the gel beads was transformed to millimeter size from the con- This research was supported by the International S&T Innovation
ventional micro-sized. This type of bead would be expected to be seen Cooperation Key Project (2017YFE0135400) and National Natural Sci-
more abundantly in combination with other foods or drinks. ence Foundation of China (32072153). The research is also supported
Another significant hindrance to food application is that most bioma- by National First-class Discipline Program of Food Science and Technol-
terials cannot withstand high temperatures and shear during processing. ogy (JUFSTR20180204) and the program of "Collaborative Innovation
As the materials for hydrogels are generally protein or polysaccharides, Center of Food Safety and Quality Control in Jiangsu Province", China.
during food processing, they undergo physical and chemical changes.
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