Trends in Food Science & Technology 98 (2020) 117–128

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Trends in Food Science & Technology

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

Phytoparticles for the stabilization of Pickering emulsions in the formulation T

of novel food colloidal dispersions
Seid Mahdi Jafaria,∗, Ali Sedaghat Doostb, Maryam Nikbakht Nasrabadic, Sareh Boostanid,
Paul Van der Meerenb
a
Department of Food Materials and Process Design Engineering, Gorgan University of Agricultural Sciences and Natural Resources, Gorgan, Iran
b
Particle and Interfacial Technology Group (PaInT), Department of Green Chemistry and Technology, Faculty of Bioscience Engineering, Ghent University, Coupure Links
653, Gent, 9000, Belgium
c
Department of Food Science and Technology, College of Agriculture, Isfahan University of Technology, Isfahan, Iran
d
Department of Food Science and Technology, College of Agriculture, Shiraz University, Shiraz, Iran

A R T I C LE I N FO A B S T R A C T

Keywords: Background: Solid particles with certain characteristics, including desired wettability, and size have been shown
Pickering stabilization as an alternative for conventional emulsifiers. They induce a form of stabilization known as Pickering to prepare
Plant-based particles emulsions. Much of the research has been conducted on the exploration of food grade particles and among those
Emulsions phytoparticles have attracted a great demand.
Biopolymers
Scope and approach: Pickering emulsions as promising delivery systems could be potentially employed for the
Novel dispersions
formulation of novel colloidal dispersions containing both lipophilic and hydrophilic bioactive compounds. In
this article, the initial focus is on the fundamental principles of Pickering stabilization followed by an overview
of recent research dealing with the fabrication of food grade Pickering emulsions stabilized by phytoparticles.
Finally, relevant food applications of such emulsions are given.
Key findings and conclusions: Plant derivatives such as proteins, polysaccharides, and their mixture as well as
waxes have been the subject of several studies to encapsulate common bioactive compounds. Plant-derived
particles have been found to effectively stabilize emulsions against different physical and chemical deteriora-
tions, including coalescence, Ostwald ripening, and lipid oxidation. These surfactant-free systems are currently
gaining an increased interest due to their techno-functional, health-promoting, economic, biocompatibility and
sustainability characteristics.

1. Introduction in personal care, medicine, agrochemical, and topical delivery products

A vast variety of food products exists in which oil and water are
present as two immiscible phases. A system to overcome this challenge
is known as an emulsion; a phase is dispersed in another in the presence
of surfactants: oil-in-water (O/W) (e.g. milk and mayonnaise), water-in-
oil (W/O) (e.g. butter and margarine), water-in-oil-in-water (W/O/W),
or oil-in-water-in-oil (O/W/O) are just some examples of emulsions
(Jafari, Beheshti, & Assadpoor, 2012, Mcclements & Jafari, 2018). They
could be an ideal delivery system for bioactive compounds, including
carotenoids, essential oils and fatty acids and some phenolic com-
pounds (e.g. curcumin) through incorporation of these added-value
compounds into the lipid or aqueous phase (Akhavan, Assadpour,
Katouzian, & Jafari, 2018; Faridi esfanjani, Assadpour, & Jafari, 2018).
Emulsions are increasingly applied not only in food products, but also
(Feng, Chen, Wu, Jafari, & Mcclements, 2018; Jafari, Paximada,
Mandala, Assadpour, & Mehrnia, 2017).
Emulsifiers are traditionally used to stabilize liquid-liquid or liquid-
gas phases by their amphoteric properties. On the other hand, much of
the recent research has been focused on biopolymers with a surface
activity. Pickering emulsions, particle-stabilized emulsions, have at-
tracted considerable interest because of their advantages over conven-
tional emulsions (Binks & Horozov, 2006; Ngai & Bon, 2015). These
surfactant-free emulsions have superior stability against coalescence in
comparison to low molecular weight emulsifiers (Pickering, 1907;
Schröder, Corstens, Ho, Schroën, & Berton-Carabin, 2018). There are
several factors that should be taken into account in the choice of a
stabilizer for a Pickering emulsion, including improving physicochem-
ical stability of the emulsion, enhanced functionality, and having a

∗
Corresponding author.
E-mail address: smjafari@gau.ac.ir (S.M. Jafari).

https://doi.org/10.1016/j.tifs.2020.02.008
Received 31 October 2019; Received in revised form 24 January 2020; Accepted 15 February 2020
Available online 20 February 2020
0924-2244/ © 2020 Elsevier Ltd. All rights reserved.
S.M. Jafari, et al.
surfactant-free label (Schröder, Corstens, et al., 2018). Inorganic or
synthetic particles such as clay, silica, and latex have been used for
Pickering stabilization of emulsions while there is growing interest in
using food-grade particles from organic and natural sources especially
for food applications (Rayner et al., 2014). One of the options for food
grade particles is plant-based particles (phytoparticles), including pro-
teins, polysaccharides, their combination, and waxes, which have
mainly no reported adverse side effects. Both O/W and W/O emulsions
can be formulated utilizing these particles with an appropriate wett-
ability, and particle size (Duffus, Norton, Smith, Norton, & Spyropoulos,
2016). In this article, we first review the basic theory of Pickering
stabilization and then provide an overview of the recent advances about
Pickering stabilization by phytoparticles. The methods to prepare the
particles and relevant food applications of these Pickering emulsions
are finally highlighted.
2. Basic principles of Pickering stabilization
In 1907, Spencer Umfreville Pickering believed that emulsions sta-
bilized using organic substances such as milk, starch, and saponin
would become spontaneously de-emulsified due to stress conditions,
including pH variation and high ionic strength (Pickering, 1907). He
reported that paraffin emulsions prepared by solid particles which were
not soluble in the oil phase and had little tendency towards the aqueous
phase, were both resistant to coalescence and did not show spontaneous
de-emulsification. Since then, emulsions stabilized using solid particles
at the interface are known as ‘Pickering emulsions’. One of the differ-
ences between Pickering emulsions and conventionally stabilized
emulsions is at their interface; Pickering stabilized oil droplets have
usually a higher surface load and thickness due to the adsorption of
particles than normal emulsions (Binks & Horozov, 2006; Ngai & Bon,
2015). Another considerable difference is the emulsifier dynamic ex-
change at the interface of conventional emulsions, not seen in Pickering
emulsions (Schmitt & Ravaine, 2013).
Any colloidal particles which can inhibit droplet coalescence and
phase separation in different types of emulsions, including, O/W, W/O,
or multiple emulsions mainly due to steric barrier can be used for the
Pickering stabilization (Rousseau, 2013). Different qualifications have
been considered for the particles to be capable of Pickering stabiliza-
tion; i.e. a) particles should not have a tendency (solubility) for neither
the hydrophobic nor the hydrophilic phases, meaning that they can be
wetted partially by both phases: theoretically, particles exerting a
contact angle of 90° at the interface are considered as the optimum b)
they should be able to efficiently adsorb at the interface, and c) typi-
cally, the size of particles is believed to be one order of magnitude
smaller than that of the ultimate emulsions (Xiao, Li, & Huang, 2016).
In fact, the free energy for detachment of a spherical particle from an
oil-water interface is expressed through the following equation:
ΔG = π r 2 γOW (1 − cos θ )2 (1)
where r is the radius of particle, γ is the oil-water interfacial tension,
and θ is the contact angle. It is obvious that the movement of a hy-
drophobic particle onto the oil phase needs a lower detachment energy
than into the water phase and vice versa for a hydrophilic particle
(Rayner et al., 2014). Thus, the free energy of a particle with a 90°
contact angle to detach into both phases is equal and thereby this
particle mainly deposits at the oil-water interface which is a pre-
requisite for Pickering stabilization. For instance, in terms of nanometer
range particles, if the detachment energy is higher than the Brownian
thermal energy of the particles, they remain at the interface.
In addition to wettability, size and shape of the particles are other
factors which could influence the formation and characteristics of
Pickering emulsions. As a rule of thumb, it has been claimed that the
size of particles should be initially about one-tenth of the desired
emulsion droplets (Sedaghat Doost, Nikbakht Nasrabadi, et al., 2019).
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Trends in Food Science & Technology 98 (2020) 117–128
However, it should be taken into consideration that the continuous
phase and the lipid phase are usually homogenized to form the emul-
sions droplets using semi-high energy methods such as high shear
(rotor-stator) homogenizers. This mixing may decrease the size dis-
tribution of particles before they can adsorb onto the interface. The
mean droplet size of emulsions is also linked to the shape of particles by
a factor defined as the aspect ratio (the length to the width ratio of a
particle). Generally, there is no control over the shape of particles and
they may take any shape depending on different parameters such as
their composition or environmental conditions such as pH and solvent
type. Particles with a higher aspect ratio have a higher capability to wet
both phases and thereby suitable for stabilization. As an example, mi-
cron-sized spindle like hematite particles with an aspect ratio of > 4.6
are an ideal case (Schröder, Corstens, et al., 2018). For a more detailed
description about the basic theory of Pickering stabilization, the readers
are referred to a book chapter by Schröder, Corstens, et al. (2018).
3. Plant-derived particles
One of the main areas of interest in recent research activities in the
field of Food Science is the exploration of proper building blocks and
appropriate fabrication methods for production of food-grade Pickering
emulsions. Two commonly used functional ingredients, which are
mostly applied for stabilizing edible Pickering emulsions, are proteins
and polysaccharides (Dickinson, 2017). Plant-based proteins and
polysaccharides offer some advantages over their animal counterparts,
including a lower risk of infection and contamination, no limitations in
terms of cultural food habits and vegetarian consumers, and more
economic advantages and versatility compared to animal-based in-
gredients (González-Pérez & Arellano, 2009, Joye & Mcclements,
2014). This section overviews the newly documented literature fo-
cusing on the plant based biopolymeric particles as appropriate Pick-
ering candidates.
3.1. Plant-derived protein particles
Proteins are composed of amino acids with various side chains and
functional groups, which imply their amphiphilic character and sub-
sequent effect as emulsion stabilizing agents. Most proteins are digested
easily within the human gastrointestinal tract (GIT), which is crucial for
the biological fate of encapsulated bioactive compounds (Yousefi &
Jafari, 2019). Moreover, proteins usually exhibit antioxidant features,
which cause a protection against chemical degradation of labile
bioactive compounds (Akbarbaglu et al., 2019; Sarabandi & Jafari,
2020). The majority of plant-based protein sources which are currently
under scientific/technological investigation or already exist on the
market are classified into legume grains such as peas, soybeans, lupins,
peanuts or chickpeas; cereals such as wheat, corn, barley, rye, sorghum,
oat or rice; oilseeds, root vegetables, leaves and fruits. Seed proteins can
be categorized into three groups of biological active proteins, structural
proteins and storage proteins (González-Pérez & Arellano, 2009). Ac-
cording to the published reports, most of the successful Pickering can-
didates based on plant proteins are found in the category of seeds/
grains storage proteins; these are categorized into four groups based on
their solubility: (1) albumins and (2) globulins are soluble in water and
diluted salt solutions, respectively; they are the main storage proteins of
dicotyledonous plants (e.g., legumes, oilseeds): whilst, (3) glutelins and
(4) prolamins on the other hand are soluble in weak alkaline/acidic and
alcoholic solutions, respectively (Boostani et al., 2019). Some of the
recent works are given in Table 1.
Soy proteins are commercially available and can be isolated from a
widely abundant and cheap source (soybeans); they exhibit health
promoting properties owing to their good nutritional value, biological
functionality, digestibility and processability (Liu & Tang, 2016a;
Zhang et al., 2018). Soy protein isolate (SPI) which has wide applica-
tions in the food industry is a mixture of various proteins mostly
S.M. Jafari, et al. Trends in Food Science & Technology 98 (2020) 117–128

Table 1
The recent studies about Pickering emulsions containing plant-derived proteins.
Particle origin Investigation Reference

Soy proteins Effect of protein concentration and/or emulsification process on emulsifying ability Liu and Tang (2014a)
Structural and emulsifying characterization of soy glycinin and effect of heat treatment on the Liu and Tang (2016a)
assembly at interface
Improvement of emulsifying ability of heat-treated soy glycinin through electrostatic screening by Liu and Tang (2016b)
addition of salt
Freeze-thaw stability of Pickering emulsions Zhu et al. (2017)
Characterization of Ca2+-induced nanoparticles Liu et al. (2017)
Characterization and emulsifying ability of ultrasound-induced soy peptide nanoparticles Zhang et al. (2018)
Soy peptides functionalized calcium phosphate for stabilization of pH switchable Pickering Ruan, Guo, Wan, Ren, and Yang (2017)
emulsion
Zein Effect of pH and ionic strength on wettability de Folter et al. (2012)
Surface modification with sodium stearate Gao et al. (2014)
Synergic effect of lecithin Rutkevičius et al. (2018)
Performance at water-water interfaces Chatsisvili et al. (2017)
Gliadin Characterization of O/W emulsions and HIPE Hu et al. (2016)
Effect of pH, ionic strength, temperature or oil content on the emulsifying ability of particles and (Zou, Van Baalen, Yang, & Scholten, 2018b), (Zhu
the rheological properties of stabilized emulsions et al., 2018a, 2018b)
Stabilizing W/O/W emulsion gels Chen, Mcclements, et al. (2018)
Wheat gluten Effect of pH, salt and temperature on Pickering emulsions Fu et al. (2019)
Kafirin Emulsifying properties of particles and rheology of emulsions in the presence of salt Xiao, Wang, et al. (2016)
Fabrication of W/O/W Pickering emulsion Xiao et al. (2017)
Hordein and secalin Physical modification of hordein and secalin particles Boostani et al. (2019)
Pea proteins O/W Pickering emulsions at pH 3 Liang and Tang (2014)
β-caroten gel-like Pickering emulsion at pH 3 Shao and Tang (2016)
Lupin protein Chemical characterization and emulsifying properties Burgos-Díaz et al. (2019)
Quinoa proteins Effect of sonication on the emulsifying ability and the effect of salt on the emulsion freeze-thaw Qin et al. (2018)
stability
Peanut proteins 5-demethylnobiletin from aged citrus peel O/W Pickering emulsions Ning et al. (2019)

globulin proteins (Nishinari, Fang, Guo, & Phillips, 2014). Soy glycinin
(SG), as the most prevalent globulin in SPI have shown a great potential
as Pickering stabilizer (Liu & Tang, 2016b). Thermal treatment of a SG
solution at 90 and 100 °C led to an increase in the particle size and
surface hydrophobicity of the nanoaggregates, indicating that the heat
pretreatment substantially improved their aggregation state. Thermal
treatment strengthened the internal integrity of the nanoparticles which
in turn enhanced their emulsifying properties owning to a pronounced
packing and diffusion at the oil and water interface (Liu & Tang,
2016a). Electrostatic screening by addition of salt was found to be re-
markably favorable for the emulsification performance of heat-treated
SG-stabilized emulsions (Liu & Tang, 2016b). As reported by Zhu,
Zhang, Lin, and Tang (2017), the freeze-thaw stability of Pickering
emulsions containing SPI was improved against coalescence and
creaming by addition of salt. This was thought to be due to the stronger
protein coating films around the droplets rather than by prevention of
ice crystal formation in the presence of salt (Zhu et al., 2017).
Proteins containing prolamins have attracted interest due to their
hydrophobic nature, unlike many other food proteins which are mostly
water soluble. Some examples are zein (corn), kafirin (sorghum),
gliadin (wheat), avenin (oat), secalin (rye) and hordein (barley)
(González-Pérez & Arellano, 2009). Their low solubility in both water
and oil phases makes them ideal for the fabrication of particles through
simple anti-solvent precipitation. Moreover, their ultimate particles
commonly do not need hardening using glutaraldehyde to enhance
their internal integrity, which subsequently simplifies the fabrication
method.
Zein is a well-known prolamin protein of corn which has been ex-
tensively studied. Many attempts have been made to commercialize its
usage in various industrial applications (Vahedikia et al., 2019). Rela-
tively monodisperse nanoparticles (~82 nm) of zein at pH values above
and below its isoelectric point (pI ~ 6.5) and low to moderate ionic
strengths readily adsorb at the oil-water interface with a contact angle
of about 90°. Changing the pH and ionic strength can influence the
hydrophilic/hydrophobic properties of the particles, causing variations
in their ability to aggregate (de Folter, Van ruijven, & Velikov, 2012).
Synergic effect of an oil soluble surfactant (lecithin) prior to
emulsification promoted the formation of emulsions with a phase in-
version point at 40 vol% of dispersed phase (Rutkevičius, Allred, Velev,
& Velikov, 2018). Colloidal particles of zein have been found to accu-
mulate at water-water interfaces with phase separating aqueous mix-
tures of fish gelatin and dextran (Chatsisvili, Philipse, Loppinet, &
Tromp, 2017). An improvement in dispersibility and interfacial char-
acteristics of zein particles by coating the particle surface with ionic
surfactants (sodium stearate) have been reported by (Gao et al., 2014).
Gliadin as prolamin-type proteins of wheat were found as effective
Pickering stabilizers for O/W emulsions as well as Pickering high in-
ternal phase emulsions (Hu et al., 2016). Gliadin particles with a size of
about 120 nm at a pH value below and above its isoelectric point
(~pH = 6.0) could stabilize O/W emulsions. Optical microscopy and
confocal laser scanning microscopy (CLSM) indicated that further to
Pickering stabilization, a dispersed droplet-based networks also caused
the stabilization of emulsions in a pH-dependent manner. The impact of
pH, ionic strength or oil content on the Pickering-stabilization behavior
of gliadin nanoparticles showed that the impact of pH and ionic
strength was attributed to their ability to alter the electrostatic inter-
actions between the gliadin nanoparticles at the interface and present in
the surrounding continuous phase. In contrast, the rheological proper-
ties of emulsions could be governed by alteration of the oil content and
electrostatic interactions (pH and ionic strength) (Zhu, Chen,
Mcclements, Zou, & Liu, 2018a; Zou, Baalen, Yang, & Scholten, 2018a).
Gliadin nanoparticles are also capable to stabilize W/O/W emulsion
gels with the presence of gliadin nanoparticles in the external aqueous
phase. This system was also successful to co-encapsulate both hydro-
philic and hydrophobic bioactive compounds (Chen, Mcclements, et al.,
2018).
Many attempts have been made recently to improve technological
and industrial applications of kafirin based products as a value-added
protein beyond animal feed (Xiao, Wang, Perez Gonzalez, & Huang,
2016). Kafirin nanoparticles demonstrated more water wetting pre-
ference with a triphasic contact angle of about 125°. The resultant O/W
emulsions resisted against coalescence. Interestingly, the addition of
salt has been shown to enhance the migration and adsorption process
through charge screening of the electrostatic interactions, thus

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S.M. Jafari, et al.
promoting the emulsifying ability as well as the stiffness of gel-like
emulsions (Xiao, Wang, et al., 2016). W/O/W Pickering double emul-
sions were also reported to be successfully formed by kafirin nano-
particles as outer layer stabilizer. However, the osmotic pressure-driven
swelling process was the major challenge for the long-term stability of
these double emulsions during storage as revealed by CLSM (Xiao, Lu, &
Huang, 2017).
Hordein and secalin are two other types of the prolamin protein
family; their ability as Pickering stabilizers is less known. Hordein is the
main prolamin of barley and has four sub-groups based on its amino
acid composition; β-hordein constitutes more than 70% of the total
barley prolamins. The high surface hydrophobicity and strong ag-
gregation behavior of β-hordein has made it a potential candidate to
adsorb at air-liquid and oil-liquid interfaces and to develop viscoelastic
films. Secalin as the storage protein of rye is structurally similar to the
corresponding wheat prolamin. However, it has been reported to have a
higher surface activity and spreading rate than gliadin. Recently,
Boostani et al. (2019) showed that a simple anti-solvent precipitation
method in combination with sonication could be applied to fabricate
submicron particles. They reported that both hordein and secalin par-
ticles show the ability to develop emulsion-foam (triphasic) Pickering
structures.
Wheat gluten is a by-product of the wheat starch industry, which is
relatively cheap and contains eight essential amino acids. Wheat gluten
is commonly used for formulating various food products owning to its
great viscoelastic features, as well as water absorption and fat-binding
properties. Wheat gluten particles were formed via a pH-cycle method
and its Pickering emulsions showed good stability over a wide range of
pH values and salt levels and thermal sterilization (Fu et al., 2019).
Other plant proteins which have recently been shown to be suitable
for producing biopolymer particles are pea legumin (Liang & Tang,
2014), protein-rich lupin variety (Burgos-Díaz et al., 2019) and quinoa
(Qin, Luo, Peng, Lu, & Zou, 2018). Pea protein isolate (PPI) is one of the
commercially available plant proteins (Liang & Tang, 2014). PPI has a
relatively small hydrodynamic diameter at pH = 3.0 and showed
Pickering stabilization for O/W emulsions which demonstrated similar
properties to numerous reported Pickering emulsions. PPI-stabilized
Pickering emulsions fabricated by microfluidization strengthened the
gel-like network by increasing the oil content, which was mostly at-
tributed to droplet flocculation and inter-floc attractive interactions
(Shao & Tang, 2016). Pickering stabilization by the protein-rich lupin
(AluProt-CGNA® variety) was investigated by Burgos-Díaz et al. (2019).
This novel non-genetically modified cultivar has a higher protein con-
tent in its dehulled seeds (about 60%) than other legumes commonly
used in the food industry. Lupin protein aggregates were fabricated via
heat-induced aggregation and showed to be effective for stabilizing O/
W Pickering emulsions.
Quinoa originates from South America and has been planted widely
in recent years owning to its significant nutritional properties. Quinoa
protein isolate (QPI) has a high content of essential amino acids and can
easily be changed to nanoparticles at pH = 7.0 (with a particle dia-
meter of about 400 nm). The sonicated QPI particles stabilized O/W
Pickering emulsions with a better emulsification efficiency, which
might be due to the stronger interparticle structures and a better sta-
bility against coalescence and coacervation (Qin et al., 2018).
3.2. Plant-based polysaccharide particles
Most of the polysaccharides, which are classified as non-adsorbing
polysaccharides, such as pectin and many gums, have been used for
stabilizing emulsions as viscosity modifiers. However, hydrophobically
modified polysaccharides and those containing proteins in their struc-
ture such as Arabic gum, also can be used as emulsifiers due to their
surface activity (Hosseini, Jafari, Mirzaei, Asghari, & Akhavan, 2015;
Shamsara, Jafari, & Muhidinov, 2017). Plant based polysaccharides as a
sustainable, available and inexpensive source of particulate emulsifiers
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Trends in Food Science & Technology 98 (2020) 117–128
have been applied in Pickering emulsion stabilization. An advantage of
polysaccharide particles is their capability of being chemically modified
for providing favorable properties (Chen, Zheng, et al., 2018).
Cellulose is the most abundant sustainable, renewable, biocompa-
tible and biodegradable biopolymer which can be derived from plants,
animals and bacteria (Gong, Wang, & Chen, 2017). It is a linear poly-
saccharide composed of D-glucopyranose units with β-1,4-glycosidic
bonds (Hemmati, Jafari, Kashaninejad, & Barani Motlagh, 2018). Cel-
lulosic particles can be used in the form of nanofibers (CNFs) and na-
nocrystals (CNCs) for the stabilization of Pickering of emulsions (Costa,
Gomes, Tibolla, Menegalli, & Cunha, 2018). However, the micro-
fibrillated cellulose is susceptible to aggregation and its length is not
controllable, which is a disadvantage for its usage as a particle stabi-
lizer. Cellulose can be transformed into the crystalline form by re-
moving amorphous parts through strong acid hydrolysis (sulfuric,
phosphoric or hydrochloric). Visanko et al. (2014) also introduced an
acid-free oxidative treatment as an alternative for acid hydrolysis
method for fabricating crystalline cellulose from cellulose fibers. Due to
the combination of high amounts of hydroxyl groups on its surface,
which is responsible for the hydrophilic nature, and hydrophobic in-
teractions arising from the crystalline organization, CNCs have an
amphiphilic nature (Hemmati et al., 2018). These surface properties
make CNCs capable to be a Pickering stabilizer. There are several
previous reports on the application of cellulose particles (CNCs and
CNFs) derived from different plant sources including sugar beet leaves
(Tamayo Tenorio, Gieteling, Nikiforidis, Boom, & Van der Goot, 2017),
wood (Gong et al., 2017), cotton and algae (Kalashnikova, Bizot,
Bertoncini, Cathala, & Capron, 2013) and banana peels (Costa et al.,
2018) for Pickering stabilization of emulsions. Modified cellulose such
as hydroxypropyl methylcellulose and ethylcellulose can also be used as
particle stabilizers (Duffus et al., 2016). Gong et al. (2017) reported
that the oxidation of CNCs with phenyl trimethyl ammonium chloride
could modify its water dispersibility for Pickering stabilizing. Pang, Liu,
Liu, Peng, and Zhang (2018) used stearoyl chloride for the surface
hydrophobization of microcrystalline cellulose for Pickering stabiliza-
tion of W/O medium and high internal phase Pickering emulsions
(HIPPEs), i.e. the emulsions with an oil content > 74% stabilized using
particles. In a different study, Chen, Guo, et al. (2018) suggested that
chemical modification using octenyl succinic anhydride (OSA) im-
proved the HIPE stabilizing ability of CNCs due to the improvement in
their surface hydrophobicity.
Starch is the second abundant, renewable and inexpensive biopo-
lymer (polysaccharide) of glucose units which is an energy source in
plants composed of two different polymers, amylose and amylopectin
(Rostamabadi, Falsafi, & Jafari, 2019b). Amylose is a linear polymer
with α-1,4 bonds and amylopectin is a branched polymer with α-1,4
and α-1,6 bonds. Starch particles can be obtained by dissolving and
precipitation, physical or chemical size reduction of large granules, or
isolating native starch granules from plant sources which have small
granules (Saari, Heravifar, Rayner, Wahlgren, & SJÖÖ, 2016). Native
starch granules are not suitable for stabilizing O/W Pickering emulsions
due to no hydrophobicity. By hydrolysis of the amorphous regions,
starch nanocrystals can be formed which have partial dual wettability
that is more suitable for Pickering stabilization purposes (Ye et al.,
2017). Dry heating is another way of enhancing the surface hydro-
phobicity of starch granules by altering the hydrophilic surface of the
granule into a hydrophobic one (Timgren, Rayner, Dejmek, Marku, &
Sjöö, 2013). Starch nanoparticles have been used successfully as a plant
based and food grade Pickering stabilizer. The size, shape and wett-
ability of these granules which is effective on the droplet size and sta-
bility of Pickering emulsions is dependent on the starch sources (Saari
et al., 2016). Different botanical sources of starch have been studied
including quinoa, corn, rice, wheat, potato, cassava, oat and waxy
varieties of rice, corn and barley. Among starch sources, the granules
from quinoa had the best emulsifying capacity due to their small size
(0.5–2 μm), monomodal size distribution and special rounded
S.M. Jafari, et al.
Table 2
Examples of Pickering stabilization using cellulose and starch particles.
Particle origin Investigation
Polysaccharides
Cellulose Nanocrystals fabricated by acid-free oxidative treatment, physicochemical
characterization
Interfacial properties of cellulose nanoparticles from sugar beet leaves
Water dispersability modification of wood-based nanocrystals with phenyl trimethyl
ammonium chloride
Cotton and algea derived nanorods
Banana peels cellulose nanofibers, high energy emulsification
Hydroxypropyl methylcellulose and ethylcellulose for O/W and W/O emulsions
Surface modification microcrystalline particles using stearoyl chloride for W/O
emulsions
Surface modification of nanocrystals using OSA
Starch Effect of source of granules on the size, shape and wettability and its influence on the
size and stability of emulsions
Fabrication of nanoparticles using non-solvent precipitation
Modification of starch granules with heat treatment or OSA
Modification of maize starch through hydrolysis
polyhedrons morphology (Timgren et al., 2013). It is reported that the
increased surface hydrophobicity of chemically modified starch with
less than 3% OSA, which is allowed in food and pharmaceutical ap-
plications, improved its emulsifying ability (Timgren et al., 2013; Ye
et al., 2017). The development and fully characterization of novel
starch-based Pickering emulsions for topical delivery of minocycline
hydrochloride (MH) was performed to increase its efficacy and safety
(Marto et al., 2019). The results revealed that these Pickering emulsions
had no toxicity on HaCat cells in the concentration range of its anti-
staphylococcal minimum inhibitory concentration (MIC). The topical
administration of MH in starch-based Pickering emulsions provides
drug-delivery directly to the infected lesion site, and leads to fast
treatment, while avoiding the side effects common in oral MH treat-
ment; so, they are a suitable carrier to be used against superficial S.
aureus skin infections. Starch-based Pickering emulsion technology
seems to be a potential candidate for further research studies and, in the
future, for expanding the pharmaceutical market of topical antibiotics
(Marto et al., 2018).
More examples of studies about stabilization of emulsions using
cellulose and starch are presented in Table 2.
3.3. Plant based protein-polysaccharide composite particles
Protein-polysaccharide interactions can be used as a source of pre-
paring bioparticles which have the combined favorable properties of
both biopolymers and their synergistic effects (Ghasemi, Jafari,
Assadpour, & Khomeiri, 2017; Moghbeli, Jafari, Maghsoudlou, &
Dehnad, 2019). Most of the plant proteins have limited applications due
to their poor solubility and sensitivity to pH, salt and temperature. The
association of a polysaccharide with these plant proteins can modulate
their functional properties especially at and around their isoelectric
point (pI). Proteins and polysaccharides can be linked together through
covalent interaction (conjugation) as a result of Maillard reaction or
non-covalent interactions (complexation) such as electrostatic interac-
tions between oppositely charged polysaccharides and proteins
(Ghasemi, Jafari, Assadpour, & Khomeiri, 2018). Maillard type reac-
tions, also called glycosylation, are known to provide permanent con-
jugates through dry or wet heating and molecular crowding of the
mixture of proteins and polysaccharides. It has been reported that
stabilized emulsions with protein-polysaccharide conjugates have a
thicker interfacial layer in comparison to emulsions stabilized by in-
dividual proteins; also, the molecular weight of applied polysaccharide
is responsible for the increase of this thickness (Akhtar & Ding, 2017).
Yang et al. (2015) reported that the obtained conjugates from the
glycosylation of soy proteins with soy polysaccharides, after reaction
for 3 days at 60 °C and 75% relative humidity, prevented coalescence in
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Trends in Food Science & Technology 98 (2020) 117–128
Reference
Visanko et al. (2014)
Tamayo Tenorio et al. (2017)
Gong et al. (2017)
Kalashnikova et al. (2013)
Costa et al. (2018)
Duffus et al. (2016)
Pang et al. (2018)
Chen, Zheng, et al. (2018b)
(GE et al., 2017; Marefati, Sjöö, Timgren, Dejmek, & Rayner, 2015;
Saari et al., 2016, 2019)
Saari, Fuentes, Sjöö, Rayner, and Wahlgren (2017)
Timgren et al. (2013)
Ye et al. (2017)
the fabricated O/W emulsion.
Electrostatic interactions can occur when oppositely charged bio-
polymers are present in the mixture, resulting in soluble or insoluble
complexes depending on the strength of the interaction (Yousefi &
Jafari, 2019). At pH values close to the pI of protein, soluble complex
particles are assembled which are stable due to their surface charge.
However, at pH values where the formed complex particles have equal
opposite charges and the net surface charge is zero, phase separation
(precipitation) between the insoluble complexes (coacervates) and
solvent occurs (Sedaghat Doost, Nikbakht Nasrabadi, et al., 2019).
There are several studies on using different protein-polysaccharide
electrostatic complexes as particulate emulsifiers. However, only a few
studies on the application of plant based complex particles for Pickering
stabilization have been published (as shown in Table 3) and most stu-
dies have been focused on complexes/conjugates of animal proteins
particularly milk proteins.
Yildiz, Ding, Andrade, Engeseth, and Feng (2018) prepared different
plant protein-polysaccharide complexes obtained from complexation
between pea or soy protein aggregates and Arabic gum, pectin, and
modified starch. All the complexes had an improved solubility around
the protein pI while the pea protein complexes had a higher solubility
and surface hydrophobicity leading to better interfacial and emulsifying
properties in comparison to soy protein complexes. Overall, based on
their results, the pea protein-starch complexes were the most suitable
particles for emulsion stabilization. Nikbakht Nasrabadi et al. (2019)
used flaxseed mucilage and flaxseed protein as biopolymers due to their
unique properties including sustainability, abundancy, and health
benefits. Their results revealed that the electrostatic interaction be-
tween flaxseed protein and mucilage was successful to overcome the pH
sensitivity of flaxseed protein and improved its Pickering emulsifying
functionality especially at and around its pI. Their CLSM and Cryo-SEM
photo analysis revealed the accumulation and adsorption of the com-
plexes onto the surface of the oil droplets (Fig. 1).
Dai, Sun, Wei, Mao, and Gao (2018) and Zhu, Lu, Zhu, Zhang, and
Yin (2019) evaluated zein nanoparticles complexed with Arabic and
corn fiber gum, respectively, as Pickering emulsifiers which were ob-
tained through the electrostatic interaction and hydrogen bonds be-
tween the gum and the fabricated zein nanoparticles by anti-solvent
precipitation. In both studies, the wettability of the zein particles was
tuned for O/W Pickering stabilization by the addition of gum. More-
over, the addition of gum to zein nanoparticles increased the particle
size and the positively charged particles became negatively charged
which was an evidence for the adsorption of gum molecules at the
surface of zein particles.
The assembly of plant proteins with polyphenols have also been
reported to improve their ability as Pickering emulsifiers and a
S.M. Jafari, et al. Trends in Food Science & Technology 98 (2020) 117–128

Table 3
Some examples of Pickering stabilization by plant protein-polysaccharide or protein-phenolic complexes.
Particle origin Investigation Reference

Protein-polysaccharide complexes
Soy protein-soy polysaccharide Maillard conjugates improved physical stability of citral emulsion Yang et al. (2015)
Soy protein-Arabic gum Effect pH and different preparation routs Kong, Jia, Zhang, Hua, and Chen
(2017)
Pea or soy protein with Arabic gum, pectin, and Physicochemical, interfacial and emulsifying properties of electrostatic complexes Yildiz et al. (2018)
modified starch
Flaxseed protein-mucilage Characterization and emulsifying properties of soluble complexes: effect of pH, Nikbakht Nasrabadi et al. (2019)
mixing ratio and total concentration
Zein-Arabic gum Characterization of Pickering emulsion gels stabilized with nanocomplexes Dai et al. (2018)
fabricated by anti-solvent precipitation
Zein-corn fiber gum Zhu et al. (2019)
Protein-polyphenol complexes
Zein-tannic acid Tuning the wettability of zein particles for stabilizing Pickering emulsion gels Zou et al. (2015)
Modification of zein particle-particle interactions and its interfacial behaviour Zou et al. (2017)
Tuning the rheology and gel strength of Pickering emulsions by tuning zein Zou et al. (2018b)
hydrophobicity effected by mixing ratio
Flaxseed protein-flaxseed polyphenols and Effect on interfacial, emulsifying and antioxidant properties of emulsions Pham et al. (2019)
hydroxytyrosol

summary of relevant studies have been presented in Table 3. Moreover,
these composites can enhance the oxidative stability of the stabilized
emulsion. It was reported that the assembly of tannic acid, as a natural
polyphenol, modified the particle-particle interactions and the inter-
facial behavior of zein nanoparticles via the hydrogen bonding of tannic
acid and the consequent decrease of the particle hydrophobicity.
Therefore, the adsorption rate of zein particles decreased, leading to a
full coverage of the stabilizing particles at the interface due to the
provided sufficient time (Zou et al., 2017). It was also reported that the
wettability of zein particles can be tuned to near neutral by this hy-
drogen bonding interaction with tannic acid which is sufficient for
Pickering stabilization of O/W emulsions (Zou, Guo, Yin, Wang, &
Yang, 2015). In a further study, it was suggested that the rheology and
the gel strength of the zein-tannic acid stabilized Pickering emulsions
can be tuned through the variation of particle hydrophobicity which
can be obtained by altering the tannic acid proportion (Zou et al.,
2018a). Recently, Pham, Wang, Zisu, and Adhikari (2019) reported that
the complexation of flaxseed protein with flaxseed polyphenols and
hydroxytyrosol improved not only the interfacial and emulsifying
ability of the protein, but also the oxidative stability of the emulsified
flaxseed oil.
3.4. Other plant-based particles
3.4.1. Cocoa particles
Cocoa particles obtained from beans of Theobroma Cacao can be
used as a food-grade particulate emulsifier. After drying, roasting,
opening of the bean and removal of the shell, the bean is separated from
the fermented pod. The removed shell is ground to prepare cocoa fiber.
Cocoa mass, a mixture of cocoa butter and cocoa particles, is obtained
by grinding the cocoa beans. Then the cocoa butter is separated using a
hydraulic press and the cocoa powder is obtained by grinding the re-
maining press cake (Joseph et al., 2019). Gould, Vieira, and Wolf
(2013) used cocoa particles obtained from different sources (cocoa
powders, cocoa fiber and cocoa mass) for the first time as a Pickering
stabilizer. Likewise, Joseph et al. (2019) investigated the effect of the
soluble and insoluble fractions of the cocoa particles on the properties
of Pickering emulsions prepared with three different emulsification
processes namely rotor/stator turbulent homogenizaion (high speed
overhead mixing), sonication and microfluidization. Their results re-
vealed that microfluidization was the most effective emulsification
process among the mentioned methods in reducing the droplet size. The
soluble and insoluble fractions of the particles did not have a significant
effect on the emulsification and stability. Table 4 provides a brief
overview of relevant studies.

Fig. 1. Cryo-SEM (a) and confocal images (b) of the flaxseed protein (FP)-soluble fraction of flaxseed mucilage (SFM) particles displayed in Rhodamine B (RB)
responsible for the stabilization of tricaprylin emulsions. Reprinted with permission from Nikbakht Nasrabadi et al. (2019).

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Table 4
Studies on the Pickering stabilized emulsions using plant-based compounds other than proteins and polysaccharides.
Particle origin Investigation Reference

Cocoa particles
Different sources (cocoa powders, cocoa fiber and cocoa mass) for Pickering stabilization Gould et al. (2013)
Effect of emulsification process and composition parameters (soluble and insoluble Joseph et al. (2019)
fractions) on O/W Pickering stabilization
Fat crystals
Glycerol monooleate Comparison of Pickering and network stabilization of W/O emulsions Ghosh et al. (2011)
Glyceryl tristearate and cetyl palmitate Esterification with citric acid to obtain glyceryl stearyl citrate Gupta and Rousseau (2012)
Glyceryl tristearate Effect of size, morphology and polymorphism on Pickering stabilization Zafeiri et al. (2017)
Tripalmitin Fate of solid lipid particles in surfactant stabilized o/w emulsions Milsmann et al. (2018)
Modification of solid lipid particles by addition of different emulsifiers Pawlik et al. (2016)
Fabrication of particles using microfluidic flow-focusing device Schröder, Sprakel, et al.
(2018)
Effect of fat based particles on lipid oxidation of the stabilized emulsions Schröder et al. (2019)
Tripalmitin, tripalmitin/tricaprylin, and palm Fabrication of particles using hot high-pressure homogenization and tuning their properties Schröder et al. (2017)
stearin for O/W emulsions
Vegetable waxes
Carnauba wax jojoba oil W/O and O/W/O emulsion Szumała and Luty (2016)
Phenolic compounds
Tiliroside, rutin and naringin Adsorption of flavonoids at the interface Luo et al. (2011)
Effect of pH on the Pickering performance of flavonoids Luo et al. (2012)
Rutin hydrate and naringin Comparison with microcrystalline cellulose, hydroxypropyl methylcellulose and Duffus et al. (2016)
ethylcellulose particles
Quercetin and curcumin Stabilizing W/O Pickering emulsions Zembyla et al. (2018)
Tea polyphenol palmitate Camellia oil W/O emulsions Luo et al. (2019)
Phytosterols
Fabrication of Particulate emulsifiers using anti-solvent precipitation Liu and Tang (2014b)

3.4.2. Fat crystals
Solid lipid nanoparticles (SLNs) are another group of plant-derived
particles which can be used as particulate emulsifiers mostly for W/O
emulsions (Katouzian, Faridi Esfanjani, Jafari, & Akhavan, 2017). Food
products such as butter, margarine, whipped cream and ice cream are
actually stabilized partially or completely by fat crystals. Fat crystals
can react as both Pickering stabilizers and network stabilizers due to
their surface activity (Zafeiri, Norton, Smith, Norton, & Spyropoulos,
2017). Surface-active fat crystals such as saturated monoacylglycerols
(MAGs) stabilize an emulsion by adsorbing at the interface and making
a protective physical barrier against coalescence while surface-inactive
fat crystals such as triacylglycerols (TAGs) stabilize oil droplets by
forming a fat crystal network (Pawlik, Kurukji, Norton, & Spyropoulos,
2016; Rousseau, 2013). Ghosh, Tran, and Rousseau (2011) reported
that the Pickering stabilization mechanism of surface-active glycerol
monooleate fat crystals was more effective in comparison to the net-
work stabilization of surface-inactive hydrogenated canola oil fat
crystals. In some cases, with sufficiently high concentration of fat
crystals, it is possible that the stabilization of emulsions is triggered by
both Pickering and network stabilization. Butter and margarine are W/
O emulsions which are normally stabilized with such a hurdle stabili-
zation mechanism.
The effectiveness of fat crystals as Pickering stabilizers is dependent
on their mean size and microstructure (morphology and polymorphism)
which is related to their source (Zafeiri et al., 2017). Since fat crystals
are not naturally amphiphilic, surfactants can be used in order to in-
crease their polarity helping them to anchor at the interface of O/W
emulsions (Milsmann, Oehlke, Schrader, Greiner, & Steffen-Heins,
2018). Surfactants have an effect on the triglyceride's crystallization
polymorphic transitions after crystallization (Zafeiri et al., 2017). An-
other way to overcome this problem is esterifying with acids to prepare
hydrophilic and anionic acid esters (Gupta & Rousseau, 2012). Gupta
and Rousseau (2012) esterified MAG with citric acid to provide glyceryl
stearyl citrate as a source of surface-active SLNs which were stable with
a 152 nm mean diameter for 6 month and were used for stabilizing O/W
emulsions with a mean droplet diameter of 459 nm. These esterified
particles adsorbed at the interface and were successful to stabilize the
emulsions while in long term storage they were dissolved or desorbed.
Schröder, Sprakel, Schroën, and Berton-Carabin (2017) used colloidal
lipid particles fabricated by hot high-pressure homogenization of high
melting point fats (tripalmitin, tripalmitin/tricaprylin, and palm
stearin) in water containing Tween 40 for stabilization of O/W emul-
sions. Their results suggested that the lipid particles of the evaluated
fats had a particular morphology which resulted in a different stabi-
lizing ability. They also suggested that these Pickering emulsions were
more effective in comparison to conventional surfactants. In another
study, Schröder, Sprakel, Schroën, Spaen, and Berton-Carabin (2018)
investigated the O/W emulsion stabilizing mechanism of lipid particles
applying a microfluidic flow-focusing device. Their results revealed that
at lower rates of particle adsorption than droplet formation during the
emulsification due to the incomplete interface coverage, droplet-dro-
plet collisions happened which resulted in coalescence and destabili-
zation. They also reported that the ability of these particles in pre-
venting lipid oxidation is limited as their results showed that the
sunflower oil in water oxidation rate in these Pickering emulsions sta-
bilized with lipid particles was the same as unconventional emulsions
stabilized with sodium caseinate (Schröder, Sprakel, Boerkamp,
Schroën, & Berton-Carabin, 2019).
Vegetable waxes are by-products of vegetable oil production which
can also be applied as W/O particle stabilizers. Szumała and Luty
(2016) studied the application of carnauba wax as a vegetable wax and
jojoba oil as a liquid wax without the presence of surfactants in stabi-
lizing W/O and O/W/O emulsions. Wax crystals at the interface pre-
vented coalescence through Pickering stabilization, whereas crystals
present in the continuous phase formed a network structure between
the oil droplets. However, the complex crystal morphology of solid fat
crystals and waxes is difficult to control, which can be a problem in
using them as particulate emulsifiers.
3.4.3. Phenolic-based particles
Phenolic compounds are naturally present in fruits, vegetables,
leaves, seeds and some foods and beverages including tea, chocolate
and wine (Zembyla, Murray, & Sarkar, 2018). Flavonoids are plant
polyphenol secondary metabolites; their consumption is associated with
prevention of several diseases (Assadpour, Jafari, & Esfanjani, 2017).
Flavonoids are known to have positive effects on animal and human

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health including antioxidant and anti-inflammatory effects (Nile, Keum,
Nile, Jalde, & Patel, 2018). Luo et al. (2011) showed for the first time
that flavonoids which are neither soluble in water nor soluble in oils,
can adsorb at the oil-water interface and stabilize O/W emulsions. Luo
et al. (2012) investigated the effect of pH on the ability of tiliroside,
rutin and naringin as particulate emulsifiers and their results displayed
that at higher pH values especially for rutin, the Pickering emulsions
had a smaller droplet size. This could be due to the fact that flavonoids
have a higher solubility and more negative surface charge at higher pH
values, which resulted in a higher surface activity. Duffus et al. (2016)
also compared food-grade particles including rutin hydrate and nar-
ingin as flavonoid particle stabilizers, along with three different mod-
ified cellulose particles namely colloidal microcrystalline cellulose,
hydroxypropyl methylcellulose and ethylcellulose particles. Their re-
sults suggested that all the evaluated particles formed green and sur-
factant-free stable W/O and O/W emulsions.
Quercus suber bark (cork) was examined for its capabilities in skin
care and, unexpectedly, it was found to stabilize Pickering emulsions
(Carriço et al., 2019). Extracts from cork oak are composed mainly of
aliphatic and phenolic compounds, including terpenes such as friedelin
and botulinum acid; tannins, namely ellagitannins; and phenolic acids
such as gallic, ellagic and protocatechic. Phenolic acids, suberin and
terpenes are known to impart antioxidant activity, which in turn inhibit
the oxidation of other molecules. The heterogeneity of its chemical
composition and its extraordinary properties make Quercus suber a
material with great potential for several industries (Carriço, Ribeiro, &
Marto, 2018). Zembyla et al. (2018) reported for the first time that
quercetin and curcumin as natural polyphenols can act as W/O Pick-
ering stabilizers. Quercetin particles according to CLSM, SEM, and op-
tical microscopy result had rod-shape crystals while curcumin particles
had a polyhedral shape. It was observed by interfacial shear viscosity
measurements that the quercetin particles anchored stronger at the
interface in comparison to curcumin particles. Some more examples can
be found in Table 4.
3.4.4. Phytosterol particles
Phytosterols are plant sterols present in fruits, cereals, and nuts with
a similar structure to cholesterol and have the ability to lower the blood
cholesterol and low-density lipoprotein (LDL). They also have an anti-
inflammatory and anti-carcinogenic effect on the human health with no
adverse effects. The application of phytosterols in food and pharma-
ceutical formulations is limited due to their poor solubility in both
water and oils. However, this property provides an opportunity of being
a Pickering emulsifier. Liu and Tang (2014b) prepared a colloidal dis-
persion of phytosterols using anti-solvent precipitation for fabrication
of Pickering emulsions.
4. Fabrication methods of plant-based particles for Pickering
emulsions
Plant particles can be produced through various methods such as
dissolution and pH adjustment (Qin et al., 2018), heating (Liu and
Tang, 2014a, 2016b), ion induced aggregation (Liu, Ou, & Tang, 2017)
and anti-solvent precipitation (de Folter et al., 2012; Hu et al., 2016).
There is a certain pH condition where proteins have no net surface
charges due to the neutralization of their functional groups known as
their isoelectric point (pI). Below this pH, some of the functional groups
are protonated and the overall surface charge of the protein is positive
whereas at higher pH values, these groups are deprotonated so that the
surface charge of protein is negative. This property of proteins in
combination with an anionic polysaccharide could be exploited to
prepare particles via electrostatic interaction between these two bio-
polymers (Sedaghat Doost, Nikbakht Nasrabadi, et al., 2019). The
carboxylic group, as a functional group of polysaccharides, has a pKa of
around two, meaning that it carries negative charges in a wide range of
pH conditions making it suitable for such an interaction. For instance,
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Trends in Food Science & Technology 98 (2020) 117–128
Sedaghat Doost, Nikbakht Nasrabadi, et al. (2019) used the soluble
fraction of flaxseed mucilage for self-assembly with flaxseed proteins
through electrostatic interaction for the stabilization of O/W Pickering
emulsions.
Basically, particles which are not initially water-soluble may be
prepared by antisolvent precipitation to become dispersible, which is an
appropriate method for the fabrication of nanoparticles from both
polysaccharides and proteins. Anti-solvent precipitation is an attractive
method for the fabrication of protein nanoparticles as there is no need
for specialized operating conditions, it is relatively cheap and can be
easily scaled up (Sedaghat Doost, Kassozi, et al., 2019). This fabrication
process basically consists of three stages. After dissolving the biopo-
lymer in proper solvents, the solvent phase (which contains the bio-
polymer) is dispersed in an anti-solvent phase (which is usually an
aqueous phase) under different mixing conditions (e.g. vortex stirring,
high-speed or high-pressure homogenization and ultrasonication), and
in the last stage, the solvent in the ultimate dispersion is removed (Xiao,
Li, et al., 2016). The anti-solvent precipitation involves several steps
including induction of supersaturation, nucleation, particle growth and
coagulation (Joye & Mcclements, 2014). Nucleation and consequent
particle growth are the driving forces that cause the spontaneous for-
mation of particles (Joye & Mcclements, 2013) which arise from the
imbalance of molecular interactions between solute, solvent, and anti-
solvent. At a certain solvent to anti-solvent ratio, the solute–solute in-
teractions are sufficiently strong which can overcome other interactions
and entropy of mixing effects, leading to precipitation. The nucleation
rate is principally significant in that it modulates the final particle
characteristics such as size, composition, and morphology. To obtain
ultrafine particles, it is necessary to assign operating conditions which
favor a rapid nucleation rate and slow particle growth (Sedaghat Doost,
Muhammad, Stevens, Dewettinck, & Van der Meeren, 2018). Some
parameters such as biopolymer concentration, solvent to antisolvent
ratio, temperature, and solubility of the polymer in the antisolvent, the
sequence of adding the solutions and also the dispersion method are the
main variables that affect nucleation (Davidov-Pardo, Joye, &
Mcclements, 2015; Sedaghat Doost, Muhammad, et al., 2018). After
particle formation, it is crucial to have strong repulsion between the
individual particles to prevent aggregation. For instance, particle sta-
bility can be further improved by cross-linking or by adsorbing other
biopolymers or surfactants onto their surface (Sedaghat Doost,
Muhammad, et al., 2018, Sedaghat Doost, Kassozi, et al., 2019).
Numerous plant-based Pickering candidates have been fabricated
using a simple antisolvent procedure. Nanoparticles of zein have been
prepared via dissolution of zein in an aqueous ethanol mixture, fol-
lowed by addition to bulk water under continuous shear conditions and
removing the extra solvent by rotary evaporation. After removing the
larger particles by centrifugation, the particles were used to stabilize O/
W emulsions (de Folter et al., 2012). In another study, Boostani et al.
(2019) produced submicron particles of hordein and secalin through
dissolution of these proteins in an ethanol mixture and subsequent
addition to bulk water under continuous stirring followed by removing
of the solvent by rotary evaporation. The ultimate particles were re-
ported to stabilize a triphasic Pickering emulsion systems. Likewise,
ethyl cellulose nanoparticles have been fabricated via an antisolvent
procedure by dissolving its powder in ethanol. Then, the ethyl cellulose
solution was dropped into a xanthan gum aqueous solution under me-
chanical stirring. Vacuum rotary evaporation and dialysis were per-
formed to remove the ethanol and xanthan separately (Wu et al., 2017).
Starch-based nanospheres were prepared via a nanoprecipitation
method by dropwise addition of water (containing modified starch in a
water-miscible organic solvent) into the polymer solution and further
removing of the solvent (Tan et al., 2014).
5. Food applications of plant-based Pickering emulsions
The utilization of these emulsions in food applications has been
S.M. Jafari, et al. Trends in Food Science & Technology 98 (2020) 117–128

widely explored in lab scale. For instance, the design and development
of multi-functional food products to fulfill modern consumer demands
like feeling outstanding sensorial features is of high importance.
However, there are no well-known commercial products in which the
use of Pickering emulsions has been claimed. There are, on the other
hand, some interesting attempts where the use of Pickering emulsions
in food products has been reported. Wang et al. (2018) introduced
cellulose nanofibers and its palm oil Pickering emulsions as fat alter-
natives for replacing 30 and 50% of the original fat of the pork-emul-
sified sausages. The formulated products showed almost comparable
sensory characteristics to the control, which makes them appropriate
for developing low fat meat products. In a different study, Yano et al.
(2017) developed gluten-free rice bread without using additives. Bread
with equal specific volume to wheat bread was obtained when rice flour
with low starch damage was used as the main ingredient. Micro-
structure monitoring of the bubble wall in the fermenting batter de-
monstrated a “stone-wall” like structure analogous to the micro-
structure of Pickering emulsions rather than that of a typical wheat
dough. Furthermore, the surface tension of the dispersed solution of
flour with low starch damage was lower than that of flour with high
starch damage suggesting a hypothetical mechanism in which Pickering
stabilization facilitated swelling of the batter/bread (Yano et al., 2017).
A brief overview of some works is given in Table 5.
Further to these examples, there are numerous reports, where
Pickering emulsions stabilized with plant-based particles were used to
encapsulate and protect bioactive ingredients, to enhance their nutri-
tional value or for oil structuring purposes (Assadpour & Jafari, 2019).
These researches open a promising route based on Pickering emulsions
in food formulations. Bioactive compounds have health benefits, in-
cluding antioxidant, anticancer, and anti-inflammatory properties.
However, their sensitivity to pH, light, and thermal treatments as well
as their hydrophobic or crystalline nature with a low water solubility
may limit their utilization in food products (Sedaghat Doost,
Muhammad, et al., 2018, Sedaghat Doost, Kassozi, et al., 2019). En-
capsulation has been extensively considered as a means of delivery for
these compounds (Esfanjani & Jafari, 2016; Rezaei, Fathi, & Jafari,
2019; Rostamabadi, Falsafi, & Jafari, 2019a). For instance, β-carotene
as the most common carotenoid with a high sensitivity to oxidation was
incorporated into Pickering emulsions produced with wheat gluten
nanoparticles or wheat gluten nanoparticle-xanthan gum complexes. In
this study, it was shown that encapsulation within Pickering emulsions
was effective at protecting β-carotene from chemical degradation
during storage (Fu et al., 2019). In a different functionality, zein-chit-
osan complex particles as a carrier for curcumin were introduced to
protect the emulsion droplets from peroxidation. The formation of an
antioxidant interface in the presence of curcumin considerably en-
hanced the oxidative stability of the emulsions (Wang et al., 2015).
In terms of encapsulation, essential oils, naturally occurring
compounds with appreciable antioxidant and antimicrobial features
(Sedaghat Doost, Devlieghere, Dirckx, & Van der Meeren, 2018,
Sedaghat Doost, Dewettinck, Devlieghere, & Van der Meeren, 2018),
need to be encapsulated due to their low water solubility, strong scent
and flavor and environmental sensitivity. Thymol as a major compound
of some essential oils was loaded into zein/gum Arabic nanoparticles-
stabilized Pickering emulsions which was able to inhibit the growth of
E. coli. Additionally, Pickering emulsions showed a controlled-release
effect on thymol due to the protective effect of the stable interfacial
layer of complex particles (Li et al., 2018).
A stable interfacial layer of Pickering candidates around the oil
droplets might make these structures suitable for designing anti-obesity
formulations. High internal phase Pickering emulsions (HIPPEs) stabi-
lized with gliadin/chitosan colloid particles showed that the fraction of
free fatty acids release was below 30% for all HIPPEs, reflecting that
HIPPEs restricted the digestion rate of the inner oil (Zhou et al., 2018).
In another study, Pickering emulsions stabilized by zein/tannic acid
complex colloidal particles also slowed down the release rate of free
fatty acids during in vitro simulated digestion (Zou et al., 2015), which
is potentially beneficial for anti-obesity purposes. Pickering emulsions
can also be used as templates to structure low-viscosity liquid vegetable
oils into soft solids and oleogels. This strategy can be achieved through
HIPPEs formulations of food-grade particles (Hu et al., 2016). HIPPEs
systems can be introduced as a good substitute for margarine for-
mulations which contain partially hydrogenated oils (PHOs) (Jiao, Shi,
Wang, & Binks, 2018). Due to the food safety hazards announced by
FDA, PHOs are not allowed to be used in food production in USA since
2018 (Zhou et al., 2018). HIPPEs templated oleogelation provide some
health beneficial effects through reducing the dietary fat amount and
controlling the fat digestibility and replacing PHOs with zero trans-fat
and less saturated fats (Hu et al., 2016; Zeng et al., 2017).
Herein are some successful examples of recent works in formulation
of HIPPEs via plant-based particles. Fairly monodispersed gliadin par-
ticles showed excellent Pickering stabilization in HIPPEs. Native soy β-
conglycinin could perform as an outstanding Pickering-type stabilizer
for O/W HIPPEs up to a dispersed phase volume fraction (ϕ) of 0.88 and
fixed protein concentration in the aqueous phase of 0.5 wt%. All the
fabricated HIPPEs were stable upon heating or storage time but very
prone to freeze-thawing (Xu, Liu, & Tang, 2019). The ternary nano-
complexes of zein, sodium caseinate, and propylene glycol alginate
showed an excellent potential to prepare gel-like Pickering emulsions
with a ϕ = 0.80 v/v (Sun, Gao, & Zhong, 2018). HIPPEs with 87%
edible oil in water were stabilized by peanut protein isolate microgel
particles (Jiao et al., 2018). The dense coating made of solid particles
around the droplets tightly stuck together and provided a barrier
against deformation which makes Pickering templates suited as a
proper strategy for structuring liquid oils and representing a novel
texture.

Table 5
A list of studies with relevant food applications of plant-based Pickering stabilized emulsions.
Particle origin Application Reference (s)

Cellulose Palm oil Pickering emulsions as fat substitute of the pork-emulsified sausages Wang et al. (2018)
Tea polyphenols Camellia oil-based W/O emulsions as fat replacer Luo et al. (2019)
Starch Gluten-free rice bread without using additives Yano et al. (2017)
Soy glycinin β-carotene encapsulation and its sustained release Liu and Tang (2016c)
Wheat gluten-xanthan β-carotene encapsulation Fu et al. (2019)
Peanut protein Encapsulation of 5-demethylnobiletin a polymethoxyflavone from aged citrus peel Ning et al. (2019)
Zein-chitosan Curcumin encapsulation Wang et al. (2015)
Zein-Arabic gum Thymol delivery for antibacterial application Li et al. (2018)
Zein-tannic acid Slowing down the fat digestion and fatty acid release for anti-obesity purposes Zou et al. (2015)
Gliadin-chitosan HIPPE for controlling oil digestion Zhou et al. (2018)
Gliadin HIPPE for oil oleogelation Hu et al. (2016)
Peanut protein HIPPE as a fat replacer in margarines Jiao et al. (2018)
Soy β-conglycinin HIPPE gels Xu et al. (2019)
Zein, sodium caseinate, and propylene glycol alginate HHIPPE gels for liquid oil structuring Sun et al. (2018)

125
S.M. Jafari, et al.
6. Conclusions and future perspective
Much research in recent years has been focused on Pickering
emulsions over conventional emulsions particularly those stabilized by
plant-based particles. Plant-derived particles have been found to ef-
fectively stabilize Pickering emulsions against different physical and
chemical deteriorations, including coalescence, Ostwald ripening, and
lipid oxidation. These surfactant-free systems are currently gaining an
increased interest due to their techno-functional, health-promoting,
economic, biocompatibility and sustainability characteristics. However,
there are no well-known commercial products in which the use of
Pickering emulsions has been claimed. One of the future research as-
pects in this area could be the exploration of commercialized systems
with desired characteristics in food products. Also, Pickering emulsions
stabilized by phytoparticles could be an ideal delivery system for
bioactive compounds, including carotenoids, essential oils and fatty
acids and some phenolic compounds (e.g. curcumin) through in-
corporation of these added-value compounds into the lipid or aqueous
phase.
Acknowledgements
The second author would like to thank particle and interfacial
technology group (PaInT) at Ghent University for providing fund to his
PhD research.
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