Trends in Food Science & Technology 106 (2020) 91–103

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Trends in Food Science & Technology

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

A review of recent progress on high internal-phase Pickering emulsions in

food science
Abdullah a, Jochen Weiss b, Talha Ahmad a, Cen Zhang a, Hui Zhang a, c, d, *
a
College of Biosystems Engineering and Food Science, Zhejiang University, Hangzhou, 310058, China
b
Department of Food Physics and Meat Science, Institute of Food Science and Biotechnology, University of Hohenheim, Garbenstrasse 21/25, 70599, Stuttgart, Germany
c
Zhejiang Key Laboratory for Agro-Food Processing, Zhejiang University, Hangzhou, 310058, China
d
Ningbo Research Institute, Zhejiang University, Ningbo, 315100, China

A R T I C L E I N F O A B S T R A C T

Keywords: Background: Interest in high internal-phase emulsions, a type of highly concentrated emulsion system, has rapidly
High internal-phase pickering emulsions increased in the food industry. However, traditional stabilizers made from inorganic particles and synthetic
Biopolymer-based particles surfactants have led to adverse health effects (e.g., interference with the normal gastrointestinal tract, gut
Food applications
microbiota, and cell toxicity), which has triggered researchers to isolate and characterize new Pickering particles
from natural sources.
Scope and approach: Biopolymer-based particles have been suggested as efficient stabilizers of high internal-phase
Pickering emulsions to satisfy consumer demand for “all natural” products and the industrial drive to provide
“clean-label” food products. In this review, the particle properties including wettability, particle size, and surface
charge, which govern the formation, microstructure characterization, and rheology of highly concentrated
emulsions, are highlighted. Recent progress with emphasis on different types of Pickering particles assembled
from biopolymers and their use in emulsions for emerging food applications are discussed.
Key findings and conclusions: High internal-phase Pickering emulsions stabilized by biopolymer-based particles
have promising food applications due to their advantages of well-controlled droplet size distribution, tailored
morphology and rheology, surfactant-free character, low toxicity, and superior stability against physical and
chemical changes as well as environmental stresses. Pickering particles are classified into three categories:
polysaccharide, protein, and complex (e.g., protein-protein, protein-polysaccharide, protein-polysaccharide-lipid,
and protein-protein-polysaccharide) particles. Recent food applications include encapsulation and controlled
release, texture design and modification, lipid oxidation reduction, and trans-fat replacement. A future
perspective concerning the fabrication of biopolymer-derived particles to promote their use in highly concen­
trated emulsions for large-scale production is proposed.

1. Introduction Traditionally, high internal-phase emulsions are stabilized by inorganic

particles (e.g., silica and titania) in combination with synthetic surfac­
A high internal-phase emulsion is defined as a highly concentrated tants (e.g., Tweens and Spans) (Barbetta & Cameron, 2004; Eskandar,
emulsion system, which has a minimum volume fraction of dispersed Simovic, & Prestidge, 2007; Ikem, Menner, & Bismarck, 2008). How­
phase over 74% (Kim et al., 2017). Unlike common emulsions, which ever, some adverse health effects, such as interference with the normal
tend to break down with time through gravitational separation, droplet gastrointestinal tract, gut microbiota, and cell toxicity (McClements &
aggregation, and Ostwald ripening (McClements & Gumus, 2016), high Xiao, 2017), have been reported with the application of such stabilizers
internal-phase emulsions have shown superior stabilities against phys­ (Chevalier & Bolzinger, 2013; Sjoo, Emek, Hall, Rayner, & Wahlgren,
ical (partial coalescence and phase separation), chemical (oxidation and 2015). Recently, biopolymer-based (e.g., protein and polysaccharide)
hydrolysis), and microbiological changes as well as environmental particles have been suggested as an alternative to overcome these lim­
conditions such as temperature, pH, and ionic strength (Ma, Zou, itations in highly concentrated edible emulsions (Huang. et al., 2019;
McClements, & Liu, 2020; Wang et al., 2020; Zhou, et al., 2018). Zhu, 2019), showing great potential to meet consumer demand for “all

* Corresponding author. College of Biosystems Engineering and Food Science, Zhejiang University, Hangzhou, 310058, China.
E-mail address: [email protected] (H. Zhang).

https://doi.org/10.1016/j.tifs.2020.10.016
Received 27 April 2020; Received in revised form 10 June 2020; Accepted 4 October 2020
Available online 6 October 2020
0924-2244/© 2020 Elsevier Ltd. All rights reserved.
Abdullah et al. Trends in Food Science & Technology 106 (2020) 91–103

natural” products and the industrial drive to provide “clean-label” food perspectives to explore novel Pickering particles and the potential of
products (Linke & Drusch, 2018; Zhu, 2019). highly concentrated edible emulsions.
As an emulsion stabilized by solid particles is called a Pickering
emulsion (Hu et al., 2016), a high internal-phase emulsion stabilized by 2. Properties of Pickering particles
solid particles is also known as a “high internal-phase Pickering emul­
sion” (Capron & Cathala, 2013; Ikem et al., 2008). The wettability, Pickering particles play a key role in the formation of emulsion
particle size, and surface charge of Pickering particles play a leading role frameworks, which leads to the creation of high internal-phase Pickering
during the formation of high internal-phase Pickering emulsions, as emulsions. The main principles for a Pickering particle to be used as a
particles can effectively adsorb and irreversibly anchor at the oil-water particulate emulsifier are as follows: (i) it should be partially wetted by
interface to prevent droplet aggregation by creating steric hindrance both phases, (ii) it should preserve intermediate wettability to achieve
(Jin et al., 2017; Wang et al., 2020; Yang, Li, & Tang, 2020). The main sufficient oil-water interface absorption, and (iii) the particle size should
advantages of Pickering stabilization include well-controlled droplet be several orders of magnitude (or at least one order) smaller for tar­
size distribution and interior particle networking, low toxicity, a geted emulsion droplets to form a protective layer around droplets to
surfactant-free character, and superior stability with enhanced shelf life prevent coalescence (Xiao, Li, & Huang, 2016; Zhu, 2019). Furthermore,
from months to even years (Fig. 1) (Jin et al., 2017; Linke & Drusch, the wettability, particle size, and surface charge of Pickering particles
2018). are important parameters to consider when choosing an efficient
In recent years, researchers have reported that high internal-phase emulsifier to stabilize high internal-phase Pickering emulsions (Binks &
Pickering emulsions can be prepared with an even higher internal- Lumsdon, 2000; Dickinson, 2010; Jin et al., 2017; Paunov et al., 2007).
phase volume (ϕdisp ≥ 0.80) at a lower particle concentration. For
example, Wang et al. (2020) prepared highly concentrated emulsions
with 80% soybean oil using 1 to 4 wt% starch particles. Zhu et al. (2020) 2.1. Particle wettability
used 0.5 wt% chitin nanofibrils to produce ultrastable gel-like emulsions
comprising 88% sunflower oil. Many studies have suggested the po­ Particle wettability defined by a three-phase contact angle (θ) is a
tential of high internal-phase Pickering emulsions in the area of key parameter in Pickering-type stabilization, which regulates the dis­
encapsulation (Dai et al., 2019; Wang et al., 2020) and controlled release tribution of particles at the oil-water interface. Thermodynamically, θ is
(Tan et al., 2017; Wei, Cheng, & Huang, 2019), partially hydrogenated interrelated with the balance of surface free energies among particle-
oil alternatives (Li et al., 2020), probiotic delivery in the gastrointestinal water, particle-oil, and oil-water interfaces (Huang. et al., 2019).
tract (Su et al., 2018), texture modification (Wijaya, Van der Meeren, Briefly, if a particle has a contact angle below 90◦ , it preferably stabilizes
Wijaya, & Patel, 2017; Yang et al., 2020), and improved oxidative sta­ the oil-in-water emulsions (i.e., hydrophilic particles). If a particle
bility (Zhou, et al., 2018). makes a contact angle above 90◦ , it preferentially stabilizes the
This review covered the recent advances in the area of high internal- water-in-oil emulsions (i.e., hydrophobic particle). To achieve firm
phase Pickering emulsions with special emphasis on different types of anchoring at the oil-water interface, the particle should form a θ value
Pickering particles assembled from biopolymers. The wettability, par­ close to 90◦ (Fig. 2) so that it can be equally immersed in both dispersed
ticle size, and surface charge of Pickering particles, which govern the and continuous phases (Albert et al., 2019; Linke & Drusch, 2018).
formation, microstructure characterization, and rheology of emulsions, A Pickering particle with a three-phase contact angle in the range of
were highlighted. Recent emerging applications related to the food in­ 30–150◦ is able to stabilize Pickering emulsions by forming delicate
dustry were discussed. The article ended with a summary of future dynamic liquid bridges (Paunov et al., 2007). These bridges are influ­
enced by the particle wettability, which governs the velocity of

Fig. 1. An overview diagram of biopolymer-based Pickering particles to be used in high internal-phase Pickering emulsions for food applications.

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Fig. 2. Adsorption of Pickering particles at the oil-water interface on the basis of wettability.

particle-particle collisions and the subsequent adhesion of particles 2.3. Surface charge
required for the rational design of Pickering emulsion formulations
(Kan, Nakamura, & Watano, 2016). Native biopolymer-based Pickering The surface charge is the distribution of ions on the particle surface
particles possess dual wettability, but the particle wettability may be that affects the interfacial region of the surrounding medium. The net
modified through physical absorption (Zhou. et al., 2018) and chemical surface charge may lead to electrostatic attractions with the opposite
modifications (Chen et al., 2018) to promote sufficient adsorption and charge of the adjacent surface. Therefore, the surface charge of a Pick­
efficient packing of Pickering particles at the oil-water interface (Binks ering particle induced by both continuous and dispersed phases, or
& Clint, 2002; Dickinson, 2012). either phase is considered the origin of strong and irreversible anchoring
For example, Zhou. et al. (2018) reported a modified wettability (θ = of Pickering stabilizers at the oil-water interface (Hu et al., 2016). It
84–87◦ ) of zein-pectin hybrid particles through the physical absorption should be noted that the impacts of particle charge on the stability and
of hydrophobic zein (110.64◦ ) with hydrophilic pectin (56.68◦ ). The performance of high internal-phase Pickering emulsions throughout the
resulting Pickering particles exhibited the potential to form high shelf life are usually regulated by pH and ionic strength.
internal-phase Pickering emulsions with a percolating 3D oil droplet The pH value strongly influences the aqueous continuous phase by
network, leading to excellent thixotropy, high viscoelasticity, and governing electrostatic and steric interactions, which are of significance
improved storage stability. In addition, Chen et al. (2018) chemically to the dispersion stability, as well as droplet aggregation and emulsion
modified the surface of cellulose nanocrystals by octenyl succinic an­ stabilization (Binks & Whitby, 2005; Rayner et al., 2014). Hu et al.
hydride, and the contact angle was changed from 51.7◦ to 85◦ with an (2016) reported that an optimum pH value of 5.0 was required for
ideal wettability, resulting in gel-like high internal-phase Pickering gliadin colloidal particles to stabilize high internal-phase Pickering
emulsions at a very low concentration of 0.1 wt%. emulsions. When the pH was increased to 9.0, visual sedimentation
through particle agglomeration was observed. Wijaya et al. (2017) re­
2.2. Particle size ported that a pH value close to the isoelectric point (pH = 4.8) of whey
protein isolate particles caused severe aggregation, resulting in poor
The particle size of Pickering stabilizers is also crucial in the for­ stability of the concentrated Pickering emulsions.
mation of particle networks to develop Pickering emulsion framework. The surface charge of Pickering particles can also be modified by the
Smaller Pickering particles are preferred compared to larger ones that addition of salts, which can promote particle adsorption at the oil-water
require more time to adsorb at the oil-water interface, ultimately pro­ interface by forming a physical barrier in the form of a film. The film
ducing emulsions with large droplets. For efficient stabilization, the thickness may be varied by changing the salt concentration. If the film is
Pickering particle size must be at least one order smaller in magnitude thicker, it creates more repulsion between droplets; thus, the emulsion
than the targeted size of the emulsion droplets (Jin et al., 2017; Xiao stability is enhanced (Rayner et al., 2014). Recently, Dai et al. (2019)
et al., 2016; Zhu, 2019). reported that high internal-phase Pickering emulsions stabilized by
Recently, Wang et al. (2020) prepared 2-hydroxy-3-butoxypropyl zein-propylene glycol alginate-rhamnolipid complex particles were
starch Pickering particles with an average size of 120 nm by nano­ produced in a liquid-state at low levels of NaCl (<10 mM), but
precipitation. The irregularly shaped Pickering particles were effective increasing the concentration up to 100 mM facilitated the conversion of
in encapsulating 80% soybean oil at a concentration of 0.5 wt%, and an emulsions into a gel-like solid-state. It was suggested that the addition of
increase in the particle concentration reduced the droplet size of the NaCl reduced the electrostatic repulsion but enhanced the strength of
highly concentrated emulsions. Hu et al. (2016) developed gliadin attractive forces between the Pickering particles, which developed a 3D
colloid particles with an average diameter of 120 nm by antisolvent network in the continuous phase. Likewise, Perrin, Bizot, Cathala, and
precipitation to fabricate high internal-phase Pickering emulsions as an Capron (2014) prepared high internal-phase Pickering emulsions sta­
alternative to partially hydrogenated oils. The spherical particles bilized by chitin nanocrystals, and a soft gel was obtained but remained
showed an outstanding capacity of encapsulating 80% corn oil at a cohesive at a low ionic strength (NaCl) of 50 mM. However, by
concentration of 2 wt%. Likewise, Tan, Sun, Lin, Mu, and Ngai (2014) increasing the ionic strength to 100 mM, the gel could no longer flow on
developed spherical gelatin Pickering particles with a diameter of 200 the glass surface by virtue of its solid texture.
nm through desolvation method, which presented excellent stabilization
via adsorption and anchoring irreversibly at the oil-water interface at a 3. Materials of pickering particles
very low concentration of 0.5 wt%. By increasing the particle concen­
tration up to 1.5 wt%, the emulsion with 80% sunflower oil showed a To date, the Pickering particles obtained from polysaccharides,
more solid-like structure and remained highly stable even after 90 days proteins, and their complexes have attracted profound interest in the
of storage at ambient temperature. area of edible emulsions (Tavernier, Wijaya, Van der Meeren, Dew­
ettinck, & Patel, 2016). The biopolymer-based particles used to stabilize

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high internal-phase Pickering emulsions are classified into three cate­ modifications (Yang et al., 2018) to extend the application of Pickering
gories (Table 1): (i) polysaccharide Pickering particles, e.g., cellulose, particles to highly concentrated edible emulsions.
chitin, and starch nanocrystals; (ii) protein Pickering particles, e.g.,
gelatin, gluten, soy, and albumin proteins; and (iii) complex Pickering 3.1.1. Cellulose
particles, e.g., gliadin-chitosan, ovotransferrin-lysozyme, and Cellulose is a biocompatible and biodegradable polymer consisting
zein-sodium caseinate-propylene glycol alginate. Compared to poly­ of 1,4-D-glucopyranose units covalently bonded together through β-1,4-
saccharide particles, more recent studies have focused on protein-based glycosidic linkages. In nature, it is the most abundantly available poly­
Pickering particles, which are considered more efficient stabilizers due saccharide in many types of biomasses (e.g., trees, microorganisms, and
to their amphiphilic nature (Hao, Peng, & Tang, 2020). tunicates) (Rehman et al., 2020). Native cellulose molecules exist as
bundles of microfibrillated cellulose with highly ordered and disordered
3.1. Polysaccharides regions; i.e., crystalline and amorphous phases are interchangeably
present. These crystalline and amorphous domains can be separated
Polysaccharides are biopolymers composed of one or more types of through chemical or mechanical means, or combination of these pro­
monosaccharide units bound together through glycosidic bonds. These cesses, yielding micro, and nanocellulosic materials, such as cellulose
macromolecules vary in structure (linear or branched), degree of nanocrystals used for Pickering stabilization (Capron & Cathala, 2013;
branching, molar mass, polarity, electrical charge and degree of hy­ Tingaut, Zimmermann, & Sèbe, 2012). The methods of acid hydrolysis
drophobicity, which govern the physicochemical and functional prop­ and octenyl succinic anhydride (OSA) modifications have been
erties of the material (Haiming, Qi, Zhao, Chi, & Cheng, 2019). Native commonly used to eliminate amorphous regions from microfibrils,
polysaccharide biopolymers (e.g., cellulose, chitin, and starch) are not leading to substantially charged particle surfaces with increased hy­
ideal stabilizers, so modifications are needed to induce sufficient particle drophilicity (Azizi Samir, Alloin, & Dufresne, 2005; Chen et al., 2018).
charges by solvent precipitation (Wang et al., 2020) and chemical Among the cellulose Pickering particles, cellulose nanocrystals

Fig. 3. Fabrication of OSA-modified cellulose nanocrystals (A), of rod-like shape observed under Atomic Force Microscopy (B), for preparing stable gel-like high
internal-phase Pickering emulsions with 80% soy oil (C) (Chen et al., 2018).

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possess a more hydrophilic character that facilitates dispersion in the and neutral amino acids in polypeptide chains that regulate electric
aqueous phase and produces high internal-phase Pickering emulsions. features at different pH and salt concentrations (Damodaran, 2005; Lam
Capron and Cathala (2013) used 0.1 wt% cellulose nanocrystals to & Nickerson, 2013). Protein Pickering particles can stabilize highly
prepare ultrastable highly concentrated emulsions with an organic concentrated emulsions by creating a physical barrier among the drop­
(hexadecane/cyclohexane) phase volume fraction of 90%. The rod-like lets due to steric and electrostatic repulsive interactions (Hao et al.,
Pickering colloidal particles were prepared through acid hydrolysis, 2020; McClements, 2015; Wilde, Mackie, Husband, Gunning, & Morris,
which irreversibly adsorbed and anchored at the oil-water interface. 2004). To date, plant proteins are more commonly utilized in high
Chen et al. (2018) utilized OSA-surface modified rod-like cellulose internal-phase Pickering emulsions than animal proteins (Huang. et al.,
nanocrystals at a concentration of 0.1 wt% to form gel-like high 2019). The various techniques to prepare protein Pickering particles
internal-phase Pickering emulsions with 80% soy oil. The droplet size include centrifugation (Li et al., 2020), pH adjustment (Xu, Liu, & Tang,
and viscosity of the emulsions were easily tuned by varying the con­ 2019), dissolution (Liu, Zheng, Huang, Tang, & Ou, 2018), heat treat­
centration of OSA-modified cellulose nanocrystals (Fig. 3), suggesting ment (Su et al., 2018), desolvation (Tan, Tu, Jia, Gou, & Ngai, 2018),
possible applications for texture design and modification in food emul­ and antisolvent precipitation (Hu et al., 2016).
sion formulations.
3.2.1. Gelatin
3.1.2. Starch Gelatin is an amphiphilic biopolymer with biocompatible and
Starch is a hydrophilic biopolymer with a high molecular weight, biodegradable properties, as it is usually derived from collagen through
comprising glucose units linked together through glycosidic linkages, hydrolysis from animal sources (e.g., skin, connective tissues, and bones)
and can be frequently found in crops such as cereals, legumes, and tubers (Pal, Bajpai, & Bajpai, 2018; Rehman et al., 2020). Tan et al. (2014)
(Li Li et al., 2019). Generally, a starch molecule is composed of reported that gelatin particles (~200 nm) prepared by the desolvation
amylopectin (75–80%) and amylose (20–25%) polymers (Haiming et al., method presented excellent Pickering-type stabilization, which inhibi­
2019; Rehman et al., 2020). Native starch molecules are not ideal ted droplet coalescence at a very low concentration of 0.5 wt%. With
emulsifiers, and methods such as nanoprecipitation (Wang et al., 2020) increasing particle concentration, a more solid-like gel formed that
and acid hydrolysis (Yang et al., 2018) have been used for modifications maintained stability after storage for 90 days. Later, the group used
to extend their use in food emulsions, and offer advantages in terms of gelatin particles to stabilize 80% sunflower oil at concentrations of
better emulsification performance, good interfacial properties, and 0.3–1.5 wt%. The lipophilic substance (β-carotene) encapsulated in the
resistance against environmental stresses (Yusoff & Murray, 2011). emulsions has shown a very high retention of 90% compared to bulk oil
During the modification process, sufficient hydrophobicity should be (8%) after 27 days of storage (Tan et al., 2017). Recently, gelatin
generated on hydrophilic starch particles, which can enhance the starch- nanoparticles developed by the two-step desolvation method were used
oil affinity to improve the stability of emulsions (Rayner, Timgren, Sjöö, to form high internal-phase Pickering emulsions with a smooth porosity
& Dejmek, 2012; Timgren, Rayner, Sjöö, & Dejmek, 2011). Recently, and textured structures. The porous scaffolds prepared from these
Wang et al. (2020) prepared starch particles by nanoprecipitation to emulsions showed good cell adhesion and proliferation, indicating the
form stable high internal-phase Pickering emulsions with 80% soybean potential to be explored in tissue engineering (Tan et al., 2018).
oil. The increase in the particle concentration (e.g., 0.5, 1, 2, and 4 wt%)
induced a progressive reduction in emulsion droplet size (11.14, 8.22, 3.2.2. Gluten
6.68, and 5.89 μm). Yang et al. (2018) used 1 wt% starch nanocrystals Wheat gluten is a cysteine-rich protein obtained from wheat flour,
produced by acid hydrolysis to prepare stable emulsions with a high comprising gliadin and glutenin components connected through non­
internal phase volume (ϕdisp=0.75–0.85). The results showed that covalent (e.g., hydrophobic and hydrogen) interactions. Disulfide cross-
increasing the concentration of starch nanocrystals resulted in gel-like linking plays a main role in the formation of the interfacial particle
high internal-phase Pickering emulsions with stronger stiffness and network needed to stabilize oil droplets (Liu, Liu, Guo, Yin, & Yang,
decreased droplet size. 2017). Recently, Liu. et al. (2018) prepared wheat gluten particles via
simple dissolution to form high internal-phase Pickering emulsions as
3.1.3. Chitin mayonnaise substitutes by encapsulating 75% sunflower oil at a particle
Chitin is a biodegradable water insoluble polysaccharide comprising concentration of 1 wt% (Fig. 4). Like mayonnaise, the emulsions showed
N-acetyl glucosamine units covalently bonded via β-1,4-glycosidic similar texture properties, such as sliminess, creaminess, and smooth­
bonds (Albert et al., 2019). It is the second largest biopolymer ness. However, a much better thermal stability at 90 ◦ C for 30 min
commonly found in insects, arachnids, crustaceans, and fungi (Hamed, without apparent changes was found compared to mayonnaise, which
Ozogul, & Regenstein, 2016). Normally, chitin polymers need to be showed a total collapse.
modified before use in high internal-phase Pickering emulsions (Zhu Gliadin, as a cereal storage protein with an amphiphilic nature, is
et al., 2020). capable of forming numerous nanostructures as a potential Pickering
Perrin et al. (2014) used chitin nanocrystals developed by acid hy­ emulsifier. Hu et al. (2016) developed gliadin colloid particles through
drolysis to stabilize highly concentrated emulsions with an oil fraction antisolvent precipitation to form Pickering emulsions by stabilizing 80%
range of 75–96%. A soft gel was obtained at a particle concentration of corn oil. The emulsions showed extraordinary stability by forming a
1.5 wt%, while a semisolid viscoelastic gel was created at a higher particle network along with dispersed droplets at pH 5 and remained
concentration of 3.0 wt%. Furthermore, by increasing the NaCl con­ highly stable over 5 months of storage in a semisolid state without signs
centration from 50 to 100 mM, the emulsion structure was changed into of oiling off. It was suggested that this technique could be used to
a thick gel-like texture. Recently, Zhu et al. (2020) developed chitin transform partially hydrogenated liquid oils into viscoelastic gels as a
nanofibrils by subjecting deacetylated chitin to surface cationization, substitute for trans-fats or saturated fats.
which stabilized high internal-phase Pickering emulsions containing
88% sunflower oil at a concentration of 0.5 wt%. The formed emulsions 3.2.3. Peanut protein
were more stable at pH values between 3 and 5, and visual appearance The peanut is a main food crop consumed all over the world. Peanut
was maintained after 90 days of storage. seeds are a rich source of edible oil and especially health-promoting
proteins. For this reason, researchers have exhibited profound interest
3.2. Proteins in developing Pickering particles from peanut proteins with potential
applications in edible emulsions (Jiao, Shi, Wang, & Binks, 2018).
Proteins are amphiphilic molecules consisting of anionic, cationic Recently, spherical-shaped peanut protein isolate microgel particles

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Fig. 4. CLSM images of wheat gluten particles (A), and high internal-phase Pickering emulsions: protein particles stained with Nile Blue (B), and sunflower oil
stained with Nile Red (C) (Liu, Guo, et al., 2018). (For interpretation of the references to colour in this figure legend, the reader is referred to the Web version of
this article.)

were prepared by a two-step process of transglutamination followed by %. The emulsions were suggested to be used for the production of hi­
gel crushing, with diameters ranging from 40 to 150 nm. The microgel erarchical porous materials for potential applications in the biomedical
particles at a concentration of 1.5 wt% efficiently stabilized the high field.
internal-phase Pickering emulsions with 85% peanut oil. The emulsions In a recent study reported by Xu, Tang, and Binks (2020), bovine
showed a cream-like homogeneous appearance by trapping oil droplets serum albumin was glycated with galactose via the Maillard reaction to
into a 3D structure developed by the particles in aqueous continuous stabilize high internal-phase Pickering emulsions by encapsulating 80%
phase, which prevented droplet coalescence through steric hindrance. dodecane at a very low concentration of 0.1 wt%. The glycation
However, the emulsions formed at pH 3.0 had a larger droplet size strengthened the structural integrity and refolding ability of the stabi­
(5–50 mm) compared to the size (1–20 mm) of those formed at pH 9.0, lizer by forming a core-shell structure, which had hydrophilic moieties
which were proven to be a better substitute for partially hydrogenated (carbohydrate) on the exterior that properly covered the protein mole­
oils (Jiao et al., 2018). cules. The glycated protein particles contributed to the formation of
gel-like emulsions with excellent stability against coalescence during
3.2.4. Soy protein storage for 90 days or heating at 100 ◦ C for 15 min (Xu et al., 2020).
Soy β-conglycinin and soy glycinin are the major globulins of soy
protein obtained from soybean flour. Compared to glycinin, β-con­ 3.2.6. Whey protein
glycinin has been considered a better stabilizer due to its high structural Whey protein, a food-grade GRAS globular protein mainly consisting
stability at the oil-water interface against aggregation (Hao et al., 2020). of β-lactoglobulin and α-lactalbumin, is a byproduct obtained during the
Xu et al. (2019) developed β-conglycinin particles by pH adjustment, process of cheese-making (Ramos et al., 2019, pp. 69–100). Recently,
which demonstrated an excellent ability at a concentration of 0.2 wt% to Zamani, Malchione, Selig, and Abbaspourrad (2018) developed whey
form stable gel-like highly concentrated emulsions with 80% dodecane. protein microgels by thermal denaturation (85 ◦ C for 15 min) of whey
With an increasing particle concentration from 0.2 to 1 wt%, a pro­ protein isolates to prepare high internal-phase Pickering emulsions.
gressive decrease in the droplet size from 60 to 24 μm occurred. The Compared to the emulsions made from the nongelled whey proteins, the
formed emulsions showed outstanding stability against heating at emulsions showed a considerably longer shelf life, higher thermal sta­
100 ◦ C for 15 min, as well as during a storage period of two months. bility, and substantially improved viscoelastic properties, such as critical
Recently, Hao et al. (2020) used heat treatment to prepare soy glycinin stress, yield stress, complex modulus and elastic modulus. In another
Pickering particles, which stabilized high internal-phase Pickering study (Su et al., 2018), whey protein isolate microgels fabricated by
emulsions with 80% soy oil at a concentration of 1 wt%. The emulsions thermal treatment were used to form high internal-phase Pickering
presented excellent stability against coalescence during long-term stor­ emulsions for the purpose of protecting intestinal microflora, such as
age, and the structural integrity of soy glycinin was well maintained (no probiotics (Lactobacillus plantarum) during pasteurization. The results
aggregation at the interface or in the solution) after adsorption at the showed that the microgel-based emulsions significantly enhanced the
oil-water interface. L. plantarum viability (7 CFU/mL) after pasteurization compared with
the emulsions without microgels (3 CFU/mL). Moreover, the probiotic
3.2.5. Albumin proteins viability could also be increased by increasing the microgel concentra­
Albumin proteins are native globular proteins obtained from animal tion in highly concentrated edible emulsions.
sources and possess a compact structure in which polar groups are
located at the exterior, while nonpolar groups are present within the 3.3. Complex particles
interior (Tcholakova, Denkov, & Lips, 2008). Xu, Tang, Liu, and Liu
(2018) prepared ovalbumin Pickering particles through pH adjustment, Complex colloidal particles developed from proteins and/or poly­
which showed an outstanding ability to form ultrastable high saccharides have been proven to be more efficient Pickering emulsifiers
internal-phase Pickering emulsions. The emulsions were produced (Ma et al., 2020; Wijaya et al., 2017). For example, the protein
through a facile one-pot homogenization process using 0.2 wt% oval­ component plays a role in producing fine droplets during homogeniza­
bumin particles, and presented extraordinary stability against coales­ tion, whereas the polysaccharide component contributes to better sta­
cence, improved oxidative stability, and inhibition of volatile oil bility against environmental stresses (e.g., temperature, pH, and ionic
vaporization during prolonged heating. Earlier, Li, Xiao, Wang, and Ngai strength). The colloidal combinations may include: (i) protein-protein
(2013) developed pure bovine serum albumin nanoparticles through complexes (Wei et al., 2019); (ii) protein-polysaccharide complexes
desolvation and successfully produced high internal-phase Pickering (Huang, et al., 2019; Yang et al., 2020); and (iii) ternary complexes, such
emulsions with 80% hexane oil at particle concentrations of 0.15–2.5 wt as protein-polysaccharide-lipid (Dai et al., 2019) and

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protein-protein-polysaccharide complexes (Sun, Gao, & Zhong, 2018). excellent thixotropy (>91%). The particles imparted ideal stability to
These complex Pickering stabilizers can be formed using various ap­ emulsions against oxidation and effectively protected encapsulated
proaches, such as ultrasonication (Yang et al., 2020), electrostatic in­ curcumin from degradation induced by UV rays (Zhou. et al., 2018).
teractions (Huang, et al., 2019), solvent evaporation (Dai et al., 2019), Recently, Yang et al. (2020) prepared unique polysaccharide-protein
antisolvent precipitation (Zeng et al., 2017; Zou, Yang, & Scholten, hybrid nanoparticles with a diameter of 160 nm by ultrasonication from
2019), pH adjustment (Liu. et al., 2018; Sun et al., 2018), facile aqueous Okara to stabilize emulsions over a broad range of pH values (2.0–12.0)
dispersion (Wijaya et al., 2017), and a two-step process of trans­ and ionic strengths (0–500 mM), and the formed emulsions showed
glutamination followed by gel crushing (Jiao et al., 2018). excellent heat stability over a wide range of temperatures (50–90 ◦ C). It
was observed that the particle networking was strengthened along with
3.3.1. Protein-polysaccharide complex a progressive decrease in droplet size by increasing the particle con­
Protein-polysaccharide complex particles can better stabilize highly centration from 0.25 to 1.5 wt%. Wijaya et al. (2017) developed whey
concentrated emulsions than individual components (Wei et al., 2019; protein isolate and low methoxyl pectin complexes by simple dissolu­
Xu et al., 2020; Zhou. et al., 2018) due to the formation of an inter­ tion, which enhanced the stability of high internal-phase Pickering
polyelectrolyte framework between droplets and the intermixed layer of emulsions against coalescence compared to uncomplexed whey pro­
protein-polysaccharide colloidal particles (Fig. 6) (Dickinson, 2008; teins. However, a pH value near the isoelectric point (pH = 3.4) of the
Wijaya et al., 2017). Emulsions have shown significant long-term sta­ complexes induced strong aggregation, leading to poor stability of the
bility in extreme temperature, pH, and ionic strength conditions, as well highly concentrated emulsions.
as during drying and freeze-thawing processes (Yang et al., 2020; Zhou.
et al., 2018), which have attracted tremendous attention in the field of 3.3.2. Protein-protein complex
edible emulsion technology (Wijaya et al., 2017; Zhou. et al., 2018). Protein-protein complexes to stabilize high internal-phase Pickering
Liu, Zheng, Huang, Tang, and Ou (2018) developed a novel partic­ emulsions can be fabricated based on electrostatic attractive forces.
ulate emulsifier of cationic bovine serum albumin covered with anionic However, very limited work has been done to develop protein-protein
cellulose nanocrystals via electrostatic interactions in aqueous solution complexes to act as Pickering particles. Wei et al. (2019) prepared
at pH 3. Noticeably, the complexes at very low concentrations (0.1–0.5 ovotransferrin-lysozyme complex particles by electrostatic interactions
wt%) resulted in extraordinarily stable gel-like high internal-phase to stabilize highly concentrated emulsions, which exhibited a decreased
Pickering emulsions with a dispersed phase volume fraction of 80%. droplet size from 81.4 to 42.4 μm upon increasing the particle concen­
Huang, et al. (2019) prepared chitosan-caseinophosphopeptide nano­ tration from 0.5 to 2.0 wt% at a fixed oil volume fraction of 75%. The
complexes through electrostatic interactions, resulting in a 3D network emulsions displayed excellent stability during long-term storage by
in high internal-phase Pickering emulsions with ideal thixotropy. The virtue of a gel-like structure, which inhibited phase separation by
complex particles formed a dense interfacial layer around the com­ trapping emulsion droplets in the continuous phase. Compared to bulk
pressed droplets, efficiently suppressed linseed oil oxidation, and oil, the complex stabilized emulsions enhanced lipolysis by 39.4% and
enhanced in vitro gastrointestinal bioaccessibility of the encapsulated the bioaccessibility of the encapsulated curcumin by 22.2%, suggesting
curcumin by 28.72%. a promising opportunity to be used as an effective delivery vehicle for
Zhou, et al. (2018) assembled gliadin-chitosan colloid particles hydrophobic nutraceuticals.
through antisolvent precipitation, which formed an interfacial layer to
stabilize 75% algae oil rich in docosahexaenoic acid to prevent lipid 3.3.3. Ternary complex
oxidation (Fig. 5). Compared to bulk oil, the encapsulated curcumin in A ternary complexation involves three biopolymer-based materials
high internal-phase Pickering emulsions showed an improved bio­ (e.g., protein-polysaccharide-lipid and protein-protein-polysaccharide)
accessibility from 2.13 to 53.61%, suggesting a promising strategy for to formulate Pickering particles for the formation of high internal-
the delivery of nutraceuticals. Likewise, gliadin-chitosan complex par­ phase Pickering emulsions (Fig. 6). The potential advantages of using
ticles were used to prepare highly concentrated emulsions containing ternary complexes include better emulsification properties (viscosity
90% hexane oil with a high porosity (>90%). The formed porous ma­ and gelling properties) and improved stability against environmental
terials showed a remarkable absorption capacity by reaching saturation stresses (pH, ionic strength, and heating) compared to the characteristics
within 3 min, indicating potential in food, biomedical and environ­ of individual applications (Dai et al., 2019). Sun et al. (2018) prepared
mental applications (Zhou, Yu, Zeng, Yin, & Yang, 2019). Similarly, zein-sodium caseinate-propylene glycol alginate complex particles,
zein-pectin hybrid particles stabilized the emulsions with 80% corn oil which stabilized highly concentrated emulsions with 80% soybean oil at
at a particle concentration of 2 wt% with high viscoelasticity and a concentration of 1 wt%. The formation of ternary nanocomplexes

Fig. 5. SEM images of gliadin-chitosan complex particles (A), and CLSM images of high internal-phase Pickering emulsions: complex particles stained with Nile Blue
(B), and algae oil stained with Nile Red (C) (Zhou, et al., 2018). (For interpretation of the references to colour in this figure legend, the reader is referred to the Web
version of this article.)

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Fig. 6. Schematic representation of oil droplets stabilized by food-grade biopolymer-based Pickering particles: Polysaccharide particles (A); Protein particles (B);
Glycated-protein particles (C); Protein-polysaccharide complex particles (D); Protein-protein complex particles (E); and Ternary (protein-polysaccharide-lipid or
protein-protein-polysaccharide) complex particles (F).

involved hydrogen bonding, hydrophobic and/or electrostatic in­ surfaces at concentrations of 1–2 wt%. The produced high
teractions, which were greatly affected by the sodium caseinate con­ internal-phase Pickering emulsions exhibited smaller oil droplet sizes
centration. The nanocomplex-based emulsions showed a gel-like (<20 μm) and enhanced stability against coalescence at a wider range of
structure with a mayonnaise-like appearance. Dai et al. (2019) fabri­ pH values (4–9), temperatures (50–90 ◦ C), and NaCl concentrations
cated zein-propylene glycol alginate-rhamnolipid complex particles by (0–100 mM), indicating promising potential for food applications such
solvent evaporation, which formed a dense layer around oil droplet as texture modification, nutraceutical encapsulation, and controlled

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release. particle concentration (Yang et al., 2020) or ionic strength (Dai et al.,
2019).
4. Food applications Liu. et al. (2018) utilized 1 wt% wheat gluten particles to produce
high internal-phase Pickering emulsions as a mayonnaise substitute and
In the field of edible emulsion technology, the use of food-grade found improved viscoelasticity and consistency by increasing the par­
Pickering particles in highly concentrated emulsions has seen remark­ ticle concentration from 2 to 3 wt%. Yang et al. (2020) prepared high
able growth with the expectations to solve the great challenges related internal-phase Pickering emulsions stabilized by insoluble soy poly­
to food processing in the industry. The creation of particle-stabilized saccharide nanoparticles and found that upon increasing the concen­
high internal-phase Pickering emulsions should be in line with legal tration from 0.25 to 1.5 wt%, the particle networking was strengthened,
requirements and industrial demands to develop safer, healthier, and and the emulsion texture became highly viscoelastic.
sustainable food products (Patel, 2018). The recent emerging applica­ Recently, Dai et al. (2019) induced a texture change from liquid to
tions of highly concentrated emulsions stabilized by biopolymer Pick­ solid-like in high internal-phase Pickering emulsions stabilized by
ering particles are summarized in this section. zein-propylene glycol alginate-rhamnolipid complex particles by the
addition of NaCl up to a concentration of 100 mM. Likewise, Perrin et al.
4.1. Encapsulation and controlled release (2014) reported that by increasing the NaCl level from 50 to 100 mM,
high internal-phase Pickering emulsions stabilized by chitin nano­
The health benefits of nutraceutical compounds that protect a person crystals showed a texture change from soft to solid-like. With the
from lifestyle-related disorders have rapidly gained attention from the increasing ionic strength, the electrostatic repulsion between the Pick­
scientific community, industries, and consumers (Chen, Remondetto, & ering particles became less effective, and the strength of attractive forces
Subirade, 2006; El Sohaimy, 2012). Unfortunately, the bioactivity and was enhanced, leading to a more viscous texture.
bioavailability of functional nutraceuticals at targeted sites within the
gastrointestinal tract is largely compromised due to environmental 4.3. Lipid oxidation reduction
stresses. There have been a few reports on highly concentrated emul­
sions stabilized by Pickering particles for encapsulation and controlled Lipid oxidation produces hydroperoxides through interactions of
release of nutraceuticals (e.g., β-carotene and curcumin) (Huang. et al., unsaturated lipids with oxygen, resulting in potentially carcinogenic and
2019; Li et al., 2020; Zhou, et al., 2018). inflammatory substances in foods (Duthie, Campbell, Bestwick, Stephen,
Tan et al. (2017) studied the in vitro digestion of β-carotene encap­ & Russell, 2013; Jacobsen, Let, Nielsen, & Meyer, 2008). Food-grade
sulated in high internal-phase Pickering emulsions stabilized by gelatin particulate emulsifiers may inhibit lipid oxidation, depending on their
particles. Compared to bulk oil, the emulsions showed a very high location, molecular properties, and environmental factors. For instance,
retention (90%) of β-carotene after 27 days of storage, which was protein colloidal particles inhibit oxidation by scavenging free radicals,
attributed to the presence of gelatin particles by retarding the diffusion chelating pro-oxidative transition metals, and obstructing metal access
of free radicals and pro-oxidants. Tan et al. (2014) also conducted in vitro at the interface by electrostatic or steric interactions by forming a dense
experiments to study the potential of these highly concentrated emul­ layer around lipid droplets (Elias, Kellerby, & Decker, 2008; Hu,
sions to deliver β-carotene. The results showed that at a low particle McClements, & Decker, 2003).
concentration of 0.5 wt%, the initial release time was 36 h, and 35% Recently, Zhou, et al. (2018) studied the oxidative stability of
β-carotene was released. In comparison, at a particle concentration of gliadin-chitosan complex stabilized high internal-phase Pickering
1.5 wt%, the initial fast release time was 14 h, and 15% β-carotene was emulsions by measuring the production of oxidant markers. Compared
released, followed by a sustained release pattern. This indicated that a to bulk oil, a remarkable decrease in oxidation product content (60%
high particle concentration might lead to a higher packing density and hydroperoxides and 50% malondialdehyde) was obtained after 14 days
the development of thicker interfacial layers that would retard the of storage at 50 ◦ C. Likewise, Huang, et al. (2019) prepared high
diffusion process of the delivered nutraceutical. internal-phase Pickering emulsions stabilized by
Probiotics can provide positive health effects by regulating the nat­ chitosan-caseinophosphopeptide nanocomplexes, which showed
ural balance of gut microflora in the human gastrointestinal tract (Ooi & reduced lipid oxidation because of the dense interfacial layer around the
Liong, 2010; Su et al., 2018). However, high temperatures and relative compressed droplets. The hydroperoxide content of primary oxidation
humidity during storage may greatly affect the viability of probiotics and the malondialdehyde content of secondary oxidation were 13 and 1
(Higl et al., 2007). Recently, whey protein isolate microgels were pre­ mmol per kg of oil in the emulsions, respectively, which were much
pared to form high internal-phase Pickering emulsions to safeguard lower than the respective contents of 450 and 20 mmol per kg in bulk oil
L. plantarum during pasteurization. Compared to emulsions without during an accelerated storage period at 60 ◦ C for 10 h.
microgels (3 CFU/mL), L. plantarum viability was significantly enhanced
(7 CFU/mL) in microgel-stabilized emulsions after pasteurization. By 4.4. Trans-fat replacement
increasing the microgel concentration, the encapsulated probiotic
viability was further increased, suggesting the promising potential of Cardiovascular disparities have been considered a major cause of
whey protein isolate microgel-based emulsions to deliver probiotics in mortality around the world by virtue of excessive trans-fat intake
the gastrointestinal tract (Su et al., 2018). (Restrepo & Rieger, 2016). Since 2018, the US Food and Drug Admin­
istration has banned the use of partially hydrogenated oils because they
4.2. Texture design and modification are a major source of trans-fats in processed foods (Patel & Dewettinck,
2016). However, high internal-phase Pickering emulsion technology
Food products made of raw materials from plants or animals by may be utilized to develop food products without trans-fats in the
processing technologies possess well-defined structures. The increasing industry.
consumer awareness and industrial campaigns for clean-label products Recently, Li et al. (2020) formed several formulations without
have challenged the use of conventional food additives (e.g., artificial trans-fats based on high internal-phase Pickering emulsions as an
emulsifiers, thickeners, and wetting agents) in food processing. The alternative to partially hydrogenated oils. The encapsulated dispersed
functional colloids used to prepare high internal-phase Pickering phases included olive oil, corn oil, soybean oil, and sunflower oil, which
emulsions may be helpful to structure safer and healthier food products. were stabilized by meat protein particles. The formed emulsions
It has been reported that the texture design and modification of highly exhibited outstanding stability during heating and freeze-thawing pro­
concentrated emulsions can be achieved by varying either the Pickering cesses. Likewise, Liu. et al. (2018) used 1 wt% wheat gluten particles to

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prepare high internal-phase Pickering emulsions containing sunflower Zhejiang University, Hangzhou, China.
oil as a mayonnaise substitute. The emulsions showed excellent thermal
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This work was financially supported by the Zhejiang Provincial Hu Yin, S.-W., Zhu, J.-H., Qi, J.-R., Guo, J., Wu, L.-Y., & Yang, X.-Q. (2016). Fabrication
Natural Science Foundation of China (LR20C200001) for Distinguished and characterization of novel Pickering emulsions and Pickering high internal
Young Scholars. Abdullah was supported by the postdoc office of the

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Development of antioxidant Pickering high internal phase emulsions (HIPEs)

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 Particle Fabrication Shape Size Particle Internal-phase
concentration volume fraction

Starch 2-hydroxy-3-butoxypropyl starch Precipitation Irregular d = 120 nm 1 - 4 wt% 80% soybean oil Encapsulation and Wang et al. (2020)
particles controlled release
Starch nanocrystals Acid hydrolysis Irregular d = 100 μm 0.5–4 wt% 85% soy oil Encapsulation and Yang et al. (2018)

Abdullah et al.
controlled release
Cellulose Cellulose nanocrystals Hydrolysis using octenyl Rod-like d = 149–169 0.3–1.2 wt% 80% soy oil Encapsulation and Chen et al. (2018)
succinic anhydride nm controlled release
Cellulose nanocrystals Acid hydrolysis Rod-like L = 189 0.1 wt% 90% hexadecane Encapsulation Capron and Cathala (2013)
W = 13 nm
Chitin Chitin nanocrystals Acid hydrolysis Elongated L = 160 3 wt% 75–96% hexadecane Encapsulation Perrin et al. (2014)
W = 16 nm
Chitin nanofibrils Surface cationization Rod-like L = 10 nm 0.5 wt% 88% sunflower oil Encapsulation Zhu et al. (2020)
Proteins Bovine serum albumin glycated with Maillard reaction Globular d = 6.5 nm 0.1 wt% 80% dodecane Texture design and Xu et al. (2020)
galactose modification
Soy glycinin glycated with soy Heating Globular d = 13.5 nm 0.3–1 wt% 80% soy oil Texture design and Hao et al. (2020)
soluble polysaccharide modification
Meat protein particles Centrifugation Globular d= 2 wt% 80% olive, corn, Trans-fat replacement Li et al. (2020)
8.21–10.94 soybean, and
μm sunflower oils
Ovalbumin particles pH adjustment Globular 2.9 × 3.5 × 0.2–3 wt% 80% dodecane Lipid oxidation Xu et al. (2018)
7.2 nm reduction
Gelatin nanoparticles De-solvation Spherical d = 236 nm 2.5–10 wt % 80% hexane Encapsulation Tan et al. (2018)
Whey protein microgels Thermal denaturation Spherical d = 90 nm 1 wt% 75% corn oil Lipid oxidation Zamani et al. (2018)
reduction
whey protein isolate microgels Heating Spherical d = 300 nm 4 & 10 wt% 80 and 90% grape Encapsulation and Su et al. (2018)
seed oil probiotics delivery
Gelatin particles De-solvation and Spherical d = 236 nm 0.3–1.5 wt% 80% sunflower oil Lipid oxidation Tan et al. (2017)
crosslinking reduction
Gelatin particles De-solvation Spherical d = ~200 nm 0.5–2 wt% 80% sunflower oil Encapsulation and Tan et al. (2014)
controlled release
Bovine serum albumin nanoparticles De-solvation Globular 14 × 4 × 14 1.5–3 wt% 80% hexane Encapsulation Li et al. (2013)
nm
Soy glycinin particles Heating Globular d = 9.7 nm 1 wt% 80% soy oil Texture design and Hao et al. (2020)
modification
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Soy β-conglycinin particles pH adjustment Globular d = 7.1 nm 0.2–1 wt% 80% dodecane Encapsulation https://www.sciencedirect.com/sci
ence/article/pii/S0268005
X18312360 Xu et al. (2019)
Wheat gluten particles Dissolution Globular d = 584 nm 1 wt% 75% sunflower oil Trans-fat replacement Liu, Zheng, et al. (2018)
Peanut protein isolate microgel Transglutamination Spherical d = 40–150 1.5 wt% 85% peanut oil, Trans-fat replacement Jiao et al. (2018)
particles followed by gel crushing nm 85% n-hexane
Gliadin colloid particles Anti-solvent precipitation Spherical d = 120 nm 2 wt% 80% corn oil Trans-fat replacement Hu et al. (2016)
Protein- unique polysaccharide-protein Ultra-sonication Spherical d = 160 nm 0.25–1.5 wt% 80% soy oil Texture design and Yang et al. (2020)
polysaccharide hybrid nanoparticles from Okara modification
complex Ovalbumin-carboxymethyl cellulose Electrostatic interactions Irregular Not available 2 - 4 wt% 80% soybean oil Encapsulation Li et al. (2020)
complex
Gliadin nanoparticles-gum arabic Anti-solvent precipitation Spherical d = 251 nm 2 wt% 85% corn oil Texture design and Ma et al. (2020)
complex modification

Trends in Food Science & Technology 106 (2020) 91–103

Chitosan-caseinophosphopeptides Electrostatic interactions Spherical d = 20 nm ~0.5 wt% 80% corn and linseed Encapsulation and Huang, et al. (2019)
nanocomplexes oils controlled release
Zein-tannic acid complex Anti-solvent precipitation Spherical d = 108 nm 2 wt% 77–87% sunflower oil Encapsulation Zou et al. (2019)
Zein-apple pectin nanoparticles Anti-solvent precipitation Spherical d = 676 nm 4 wt% 80% corn germ oil Texture design and Jiang et al. (2019)
modification
Gliadin-chitosan complex particles Anti-solvent precipitation Spherical d = 25 μm 2 wt% 80 and 90% hexane Encapsulation Huang Zhou, Yang, Yin, Tang, and
Yang (2019)
Bovine serum albumin covered with pH adjustment Needle- d = 30 nm 0.1–0.5 wt% 80% soy oil Lipid oxidation Liu, Zheng, et al. (2018)
cellulose nanocrystals like reduction
Gliadin-chitosan colloid particles Anti-solvent precipitation Spherical d = 190 nm 2 wt% 75% algae oil Lipid oxidation Zhou, et al. (2018)
reduction
Zein-pectin hybrid particles Anti-solvent precipitation Spherical d = 583 nm 2 wt% 80% corn oil Lipid oxidation Zhou, et al. (2018)
reduction
Gliadin-chitosan hybrid particles Anti-solvent precipitation Spherical d = 588 nm 0.5–2 wt% 83% corn oil Encapsulation Zeng et al. (2017)
Whey protein isolate-low methoxyl Dissolution Spherical d = 250–350 1 - 5 wt% 80% sunflower oil Texture design and Wijaya et al. (2017)
pectin complex nm modification
Whey protein isolate-low methoxyl Complex coacervation Spherical d = 829 μm 1.5 wt% 79% soybean oil Encapsulation Zhu et al. (2020)
pectin complex
Protein-protein Ovotransferrin- lysozyme particles Electrostatic interactions Globular d = 100 nm 0.5, 1 & 2 wt% 75% medium chain Encapsulation and Wei et al. (2019)
complex triglycerol oil controlled release
Protein- Zein-propylene glycol alginate- Solvent evaporation Spherical d = 504 nm 1 - 2 wt % 75% medium chain Encapsulation Dai et al. (2019)