Carbohydrate Polymers 242 (2020) 116388

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Carbohydrate Polymers
journal homepage: www.elsevier.com/locate/carbpol

Recent advances in polysaccharides stabilized emulsions for encapsulation T

and delivery of bioactive food ingredients: A review
Ruyuan Zhanga, Tarun Belwala, Li Lia, Xingyu Lina, Yanqun Xua,b, Zisheng Luoa,b,c,*
a
Zhejiang University, College of Biosystems Engineering and Food Science, Key Laboratory of Agro-Products Postharvest Handling of Ministry of Agriculture and Rural
Affairs, Zhejiang Key Laboratory for Agri-Food Processing, National-Local Joint Engineering Laboratory of Intelligent Food Technology and Equipment, Hangzhou 310058,
People’s Republic of China
b
Ningbo Research Institute, Zhejiang University, Ningbo 315100, People’s Republic of China
c
Fuli Institute of Food Science, Hangzhou 310058, People’s Republic of China

ARTICLE INFO ABSTRACT

Keywords: Many bioactive food ingredients were encapsulated in different forms to improve their stability and bioavail-
Polysaccharides ability. Emulsions have showed excellent properties in encapsulation, controlled release, and targeted delivery of
Bioactive food ingredients bioactives. Polysaccharides are widely available and have different structures with different advantages in-
Emulsions cluding non-toxic, easily digested, biocompatible and can keep stable over a wide range of pH and temperatures.
Stability
In this review, the most common polysaccharides and polysaccharide based complexes as emulsifiers to stabilize
Bioavailability
emulsions in recent ten years are described. The close relationships between the types and structures of poly-
saccharides and their emulsifying capacities are discussed. In addition, the absorption and bioavailability of
bioactive food components loaded in polysaccharide stabilized emulsions are summarized. The main goal of the
review is to emphasize the important roles of polysaccharides in stabilizing emulsions. Moreover, speculations
regarded to some issues for the further exploration and possible onward developments of polysaccharides sta-
bilized emulsions are also discussed.

1. Introduction (Vareed et al., 2008). Sensitive bioactive compounds such as poly-

A large number of food-derived bioactive components play pivotal
roles in reducing the risks of cancer (Gao et al., 2017), inflammation
(Edwards et al., 2017), diabetes (Belwal, Nabavi, Nabavi, &
Habtemariam, 2017; Oh, 2016), autoimmune (Khan et al., 2019),
obesity (Leonetti et al., 2017) and cardiovascular diseases (Rimm et al.,
2018). To produce such effective health responses, these components
should be successfully delivered to the targeted tissue/organs within a
safe and effective dose level. A varied physical and chemical properties
of bioactive components resulted in problems during its effective for-
mulation and direct use. For instance, hydrophobic bioactive com-
pounds such as curcumin have low water-solubility and bioavailability,
which limits their direct effect. Free form of curcumin was almost un-
detectable in human plasma after oral administration of 12 g curcumin
phenol are unstable and oxidized easily during storage (Sun et al.,
2018), probiotic bacteria would be easily degraded by harsh acidic
condition and enzymatic reactions from ingestion to digestion (Picone,
Bueno, Michelon, & Cunha, 2017). Some food-derived bioactive com-
pounds such as saponins exhibit bad flavor and texture, thus limiting
their use by the consumers for oral uptake (Dawid & Hofmann, 2014).
Hence, ensuring the oxidative stability and high pH resistance, in-
creasing shelf-life, masking off flavor and odor, controlled delivery and
improving bioavailability of food ingredients are of great significance.
Emulsion-based encapsulation and delivery systems have exhibited
excellent performance in protecting, controlled release, and site specific
targeted delivery of bioactive components (Kotta et al., 2012). The
absorption and bioavailability of loaded bioactive components are
closely associated with the physical and chemical stability of the

Abbreviations: AGp, arabinogalactan-peptide; DDSA, dodecenyl succinic anhydride; GP, glycoproteins; O/W emulsion, oil-in-water emulsion; W/O emulsion, water-
in-oil emulsion; AG, apricot gum; AL, alginate; CAR, ι-carrageenan; CMC, carboxymethyl cellulose; DE, degree of esterification; GA, gum Arabic; HIPEs, high internal
phase emulsions; HMP, high methoxyl pectin; HPMC, hydroxypropylmethyl cellulose; ISPS, insoluble soybean polysaccharides; LCT, long chain triglycerides; LMP,
low methoxyl pectin; LPI, lentil protein isolate; MC, methyl cellulose; MCT, medium chain triglycerides; OSA, octenyl succinic anhydride; OSQS, octenylsuccinate
quinoa starch; RG-I, rhamnogalacturonan I; RG-II, rhamnogalacturonan II; SBP, sugar beet pectin; SC, sodium caseinate; SPH, soy hull polysaccharides; SPI, soy
protein isolated; SSPS, soybean soluble polysaccharides; WPI, whey protein isolate; XG, xanthan gum
⁎
Corresponding author at: College of Biosystems Engineering and Food Science, Zhejiang University, Hangzhou 310058, People’s Republic of China.
E-mail address: luozisheng@zju.edu.cn (Z. Luo).

https://doi.org/10.1016/j.carbpol.2020.116388
Received 17 January 2020; Received in revised form 17 April 2020; Accepted 27 April 2020
Available online 23 May 2020
0144-8617/ © 2020 Elsevier Ltd. All rights reserved.
R. Zhang, et al.
Fig. 1. Schematic diagram of emulsion instability mechanisms.
emulsions. The most important factors influencing the stability, release,
absorption and bioavailability of bioactive components in various
emulsion delivery systems include oil composition and volume fraction,
structure and density of interface, droplet size and dispersion condi-
tions (Li, Xiao, & McClements, 2012; Mayer, Weiss, & McClements,
2013; Saberi, Fang, & McClements, 2013). For instance, medium chain
triglycerides (MCT) and long chain triglycerides (LCT) have been
widely used as lipid carrier to deliver food pigments, flavors and es-
sences (Dianhui et al., 2019). LCT is more suitable to deliver lipophilic
compound because it has greater solubilization and higher cellular
uptake compared to MCT (Han, Gu et al., 2019; Han, Hu et al., 2019; Lu
& Huang, 2019; Xuan, Jinfeng, Hang, & McClements, 2015). A large
number of food products are structured in oil-in-water (O/W) or water-
in-oil (W/O) emulsions in their production process or final product
forms. As shown in Fig. 1, emulsions are thermodynamically unstable
and tend to separate back into oil phase and water phase, result in
creaming, sedimentation, flocculation or coalescence. Stabilizers such
as emulsifiers, thickeners and weighting agents are usually required to
resist environmental stresses and improve emulsions shelf lives. Emul-
sifiers are of great importance to the performance of emulsion-based
food products, however, nowadays most of emulsifiers used in food-
stuffs are synthetic, including fatty alcohol ethoxylates (Martinez-
Gallegos, Bravo-Rodriguez, Jurado-Alameda, & Garcia-Lopez, 2011),
sorbitan esters (Sonwai, Podchong, & Rousseau, 2017), and sucrose
esters (Ariyaprakai, Hu, & Tran, 2019). Replacing synthetic emulsifier
with natural emulsifier has aroused great interests because of its safe
and effective advantages, thus increasing its acceptability in food pro-
ducts by consumers.
Carbohydrate is the main energy source in human diets, which can
be acquired from multiple natural resources including plants (Khatun,
Waters, & Liu, 2019), animals (Hu & Ganzle, 2019) and microbes
(Mahmood, Ali, Moghaddas Kia, & Arezou, 2019). Generally, carbo-
hydrates can be divided into polysaccharides, oligosaccharides, dis-
accharides and monosaccharide according to the number of mono-
saccharide units after hydrolysis reaction. Among them,
polysaccharides are regarded as promising biopolymer for encapsula-
tion and delivery of food derived bioactive ingredients because of their
molecular structure (Mungure, Roohinejad, Bekhit, Greiner, &
Mallikarjunan, 2018). In contrast to other three saccharides, some
natural polysaccharides such as GA, pectin and galactomannans contain
proteins or non-polar groups in their hydrophilic carbohydrate chains,
2
Carbohydrate Polymers 242 (2020) 116388
thereby possessing emulsifying properties (Dickinson, 2003). Mean-
while, polysaccharide has higher molecular weight and is more suitable
as building blocks to entrap bioactives (Milad, Martin, & McClements,
2014). Moreover, polysaccharides can form an extended network in
water phase, thus can increase the viscosity of emulsions to improve
their stability (Bai et al., 2017). Polysaccharides have been widely ap-
plied in food emulsions to deliver oil soluble flavor substances, func-
tional oils, bioactive peptides, polyphenols, carotenoids and probiotics,
which can delay lipid digestion, prolong satiety and realize target de-
livery (McClements, Bai, & Chung, 2017). Compared to proteins and
surfactants, polysaccharides can provide resistant to protease and gas-
tric acid environment. For instance, pectin is one of the most common
polysaccharides which is stable in the upper gastrointestinal tract, and
mostly digested in the colon by colonic microflora (Hailong, Ke, Dong,
& Qingrong, 2012), thus can be effectively used to deliver the bioactives
to the target sites. Nevertheless, some polysaccharides present diffi-
culties in adsorption at the interface because of their highly hydrophilic
nature and complex macromolecular conformations and structures.
Hence, these polysaccharides are usually modified with hydrophobic
group to enhance their emulsifying properties (Melanie et al., 2020).
Meanwhile, polysaccharides can interact with other substances such as
small molecule surfactants, other polysaccharides or proteins to si-
multaneously stabilize emulsions (Ma et al., 2017; Senra, Campana, &
Desbrieres, 2018; Wang, Nian et al., 2019; Wang, Ghosh, & Nickerson,
2019).
To date, emulsions for encapsulation and delivery of bioactive food
ingredients have been investigated in many studies and reviews.
However, most of reviews focused on the protein stabilized emulsions
and neglected the important roles of polysaccharides. In this review, we
put strength on the excellent abilities of polysaccharides to stabilize
emulsions and deliver food bioactive components. The most common
polysaccharides including modified starch, pectin, cellulose derivatives,
GA, chitosan, inulin and seaweed polysaccharides, and their respective
emulsifying properties are also introduced. In addition, polysaccharide
complexes as emulsifiers to stabilize emulsions are described.
Moreover, the absorption and bioavailability of bioactive food com-
ponents loaded in polysaccharides based emulsions are summarized.
Speculations regarded to some issues for the further exploration and
possible onward developments of polysaccharides stabilized emulsions
are also made.
R. Zhang, et al.
Fig. 2. (A) Classification of bioactive food ingredients (Bao et al., 2019). (B) Percentage of published papers on emulsion based systems for encapsulation and
delivery of bioactive food ingredients in recent ten years.
2. Polysaccharides as emulsifiers: types and properties
As shown in Fig. 2A, the bioactive food ingredients can be broadly
classified into polyphenols, bioactive peptides, polyunsaturated fatty
acids, vitamins, bioactive polysaccharides and minerals elements (Bao
et al., 2019). Among them, vitamins have been widely studied in
emulsion based delivery systems in recent ten years (Fig. 2B). The most
common natural emulsifiers for encapsulation and delivery of bioactive
food ingredients include proteins, phospholipids and polysaccharides.
For proteins, the pH and temperature will affect its emulsifying per-
formance. Meanwhile, some of the proteins can trigger allergic reac-
tions (Benede, Lopez-Exposito, Molina, & Lopez-Fandino, 2015;
Meinlschmidt, Schweiggert-Weisz, Brode, & Eisner, 2016). For phos-
pholipids, there are concerns about its stability and purity for emulsion
formulation (Li et al., 2015). Compared to proteins and phospholipids,
polysaccharides are widely available and have a variety of structures
with different advantages including non-toxic, easily digested, bio-
compatible and can keep stable over a wide range of pH and tem-
peratures (Grumezescu & Holban, 2018; Stephen, Phillips, & Williams,
2006; Wani et al., 2016). For instance, corn fiber gum (CFG) stabilized
emulsions loaded with lutein exhibited excellent physicochemical
properties, stabilities and in vitro bioaccessibility (Feng et al., 2017).
During storage, the loaded lutein was stable and could avoid degrada-
tion under the conditions of light and high temperature. And the
bioaccessibility of lutein was increased from 13.8%–32.4% after en-
capsulated in CFG stabilized emulsions. In addition, polysaccharides
can be modified with a series of functional groups for versatile appli-
cation (Song et al., 2015).
As shown in Fig. 3, different structures of polysaccharides exhibit
different adsorbed modes on the surface of oil droplet. In the random
polysaccharides, multiple hydrophobic anchoring points spread out
along the interface and limited lateral chains protrude to the aqueous
phase. In the graft polysaccharides, the lateral chains protrude to the
water phase to provide prominent steric stabilization. In diblock poly-
saccharides, the hydrophilic buoys provide efficient steric stabilization
(Kontogiorgos, 2019). Compared with other two polysaccharides sta-
bilized emulsions, the random polysaccharides stabilized emulsions
have lower stability due to limited steric stabilization efficiency, and
thus the oil droplets tend to aggregate by attractive forces (Ettelaie,
Murray, & James, 2003). For instance, the structure of GA is mainly
consisted of a protein fraction and approximately five carbohydrate
3
Carbohydrate Polymers 242 (2020) 116388
blocks (Al-Assaf, Sakata, McKenna, Aoki, & Phillips, 2009; Dickinson,
2003). Serine and hydroxyproline residues of protein fraction could
covalently link to carbohydrate, forming arabinogalactan–protein
complexes. The hydrophobic protein fraction could firmly anchor the
GA at the surface of oil droplet, and the hydrophilic carbohydrate
blocks could act as a strong steric barrier against flocculation and
coalescence (Dickinson, 2003). According to the stabilization me-
chanism, the emulsions can be mostly divided into O/W emulsion,
multiple emulsion, multilayer emulsion, Pickering emulsion and mi-
celle (Fig. 3). And various polysaccharides have been used to stabilize
emulsions containing food bioactive components and are discussed
below and listed in Table 1.
2.1. Modified starch
Starch is easily available, cheap, non-allergenic, GRAS (Generally
Recognized As Safe) (Zhu, 2019) and has been widely found in plenty of
plant tissues, including roots, seeds, leaves, stems and tubers. According
to the structure, starch can be divided into amylose and amylopectin.
Amylose consists of glucose residues linked by α-1,4 glycosidic bonds
while amylopectin contains main chains with α-1,4 glycosidic bonds
and side chains with α-1,6 glycosidic bonds. Starch molecules are
particularly hydrophilic due to a large number of hydroxyl groups. The
chemical modification of hydrophobic groups on starch can make it
become surface active, which is considered as an ideal material for
encapsulation and delivery of insoluble bioactive food ingredients
(Wang, Luo, Chen, Fu, & Tamer, 2020; Wang, Yang et al., 2020). For
instance, modified starch stabilized coffee emulsions could control
aroma release to some extent and could be applied for instant coffee
aroma enrichment (Lee, Liu, Wong, & Liu, 2017). According to the
chemical functional approach, the modified starch can be divided into
grafted starch, block starch and polyelectrolyte starch (Xu et al., 2019).
The hydrophobic modification of starch is mainly realized through
esterification with various hydrophobic groups such as propionate
(Hong, Cheng, Gan, Lee, & Peh, 2018; Tupa, Arroyo, Herrera, & Foresti,
2018), dodecenyl succinic anhydride (DDSA) (Shah, Soni, & Singhal,
2018; Zhou, Ren, Tong, Xie, & Liu, 2009) and octenyl succinic anhy-
dride (OSA) (Bello-Perez, Bello-Floresa, Nunez-Santiago, Coronel-
Aguilera, & Alvarez-Ramirez, 2015; Dokic, Krstonosic, & Nikolic, 2012),
which can not only make the starch amphiphilic but also reduce the
intramolecular hydrogen bond to increase solubility. OSA is one of the
R. Zhang, et al. Carbohydrate Polymers 242 (2020) 116388

Fig. 3. Schematic diagram of different types of emulsions stabilized by polysaccharides (not drawn to scale).
Figure note: a. O/W emulsion (an emulsion system whose continuous phase is aqueous and the dispersed phase is oil), b. Multiple emulsion (a complex heterogeneous
system whose dispersed phase is an emulsion and contains smaller droplets, such as W/O/W emulsion (Roohinejad, Greiner, Oey, & Wen, 2018)), c. Multilayer
emulsion (a system utilize layer-by-layer methods to stabilize emulsion (Mao & Miao, 2015)), d. Pickering emulsion (emulsion system stabilized by solid particles), e.
Micelle (a system which is formed by self-assembly of amphiphilic polymers (Owen, Chan, & Shoichet, 2012)).

most commonly used hydrophobic groups for starch modification and
the surface activity of OSA-starch is similar to whey protein (Tesch,
Gerhards, & Schubert, 2002). Compared to native kudzu starch, OSA-
modified kudzu starch could further reduce interfacial tension and ex-
hibited better emulsifying capacity (Zhao et al., 2017). The emulsifying
capacity of polysaccharide is closely related to its structure. As such,
amorphous OSA starch has a better performance as emulsifier com-
pared with granular OSA starch owing to the high rate of interfacial
adsorption, larger thickness of adsorbed layers, smaller size distribution
of the oil droplets, and excellent assembly behavior of network com-
pactness (Liu, Li, Chen, Xu, & Zhong, 2018). Moreover, the dispersion
stability of OSA modified polysaccharide is not affected by pH and can
be applied to food matrix close to the isoelectric point of proteins (Zhao,
Qi, Liu, Zeng, & Yang, 2018). With the increased level of OSA, the oil
absorption ability, emulsion stability, resistant starch levels and visc-
osities of starch increased (No & Shin, 2019).
However, the reaction between starch and OSA was sometimes
limited because of the crystal helix structure, high molecular weight
and high branch degree of starch (Tizzotti, Sweedman, Schafer, &
Gilbert, 2013). As the primary degradation product of starch, dextrin
has non-Newtonian fluid properties in solutions, shows excellent
properties including water-solubility, emulsibility, dispersibility, and
can be easier modified with OSA (Pan et al., 2019). For instance, Pan
et al. prepared an OSA modified dextrin for curcumin encapsulation
and found that the encapsulation efficiency of curcumin in dextrin
stabilized emulsion was about 57.93% while in OSA modified dextrin
stabilized emulsion the encapsulation efficiency increased to 85.41%.
Moreover, the emulsifying stability of emulsion stabilized by OSA
modified dextrin was significantly improved and could keep stable for 2
weeks in the dark at room temperature (Pan et al., 2019).
Pickering emulsion is more stable against coalescence and Ostwald
ripening compared to surfactant-stabilized emulsion (Matos et al.,
2018). Different from the adsorption mechanism of surfactants, the
solid particles do not need to be amphiphilic. Partial wetting of the solid
particles make them strongly anchor at the oil–water interface and
stabilize Pickering emulsions (Chevalier & Bolzinger, 2013). In recent
years, modified starch has been widely used in the preparation and
application of Pickering emulsion because modified starch particles can
adsorb at interface to form a barrier film, which can retard the phase
separation. Both soluble starch nanoparticle and insoluble starch na-
noparticle could be used to stabilize O/W Pickering emulsion and no
phase separation was observed even after stored for 30 days (Ye et al.,
2017). Li et al. prepared an octenylsuccinate quinoa starch (OSQS)
based Pickering emulsion and firstly used for lutein encapsulation. They
surprisingly found that when the oil volume fraction (ø) was between
30% and 60%, the emulsions were self-standing and immobile, thus
formed Pickering emulsion gel. Thick adsorbed OSQS layer could
greatly increase the inter-droplet interaction and the gel network was
greatly associated with the aggregation of oil droplets. The OSQS-
granule-stabilized Pickering emulsion gel exhibited superior storage
stability and the lutein retention could reach to 55.38% after 31 days of
storage (Li, Zhang, Li, Fu, & Huang, 2020).
2.2. Pectin
Pectin is a covalently linked plant cell wall polysaccharide rich in
galacturonic acid. The industrial sources of pectin include sugar beet,
pomace and citrus peels. The backbone of pectin is mainly composed of
homogalacturonan segments consisted of D-galacruronic acid units
linked by α-(1-4) glycosidic bond (55–65%). The side chains of pectin
consist of multiple monosaccharides including xylose, glucose, fucose,
mannose, arabinose and rhamnose, which can form rhamnogalactur-
onan I (RG-I, 20–35%) or rhamnogalacturonan II (RG-II, 0–10%).
According to the degree of esterification (DE), pectin can be divided
into high methoxyl pectin (HMP, DE ＞ 50%) and low methoxyl pectin
(LMP, DE ＜ 50%). HMP can form gels in acidic high sugar medium
while LMP can form gels in the presence of multivalent cations such as
Ca2+.
Generally, the emulsifying activities of pectin depend on the protein
moiety, acetyl and feruloyl groups, and the emulsion-stabilizing prop-
erties of pectin depend on the neutral sugar side chains of RG-I and
homogalacturonan domain (Ngouemazong, Christiaens, Shpigelman,

4
 R. Zhang, et al.

Table 1
Summarization of polysaccharide stabilized emulsions for encapsulation and delivery of bioactive food ingredients.
Polysaccharide Source Modified reagent or method Bioactive food Type of Ratio of oil Polysaccharide Preparation conditions Droplet size References
ingredients emulsion phase concentration

Starch Kudzu OSA Soybean oil O/W emulsion 10% (w/w) 1–5% (w/w) 90 °C, pH 2−8, 10,000 183 to 267 nm (Zhao et al., 2017)
rpm for 5 min
Starch Waxy maize OSA MCT O/W emulsion 10% (w/w) 1% (w/w) 18,000 rpm for 5 min 283.9 nm (Liu et al., 2018)
Dextrin Corn starch OSA Curcumin in corn oil O/W emulsion 10% (w/w) 2% (w/w) 25 °C, 12,000 rpm for 4 to 6 μm (Pan et al., 2019)
2 min
Starch Quinoa OSA Resveratrol in orange oil O/W Pickering 10% (w/w) Not mention Not mention 50 μm (Matos et al.,
emulsion 2018)
Starch Waxy maize OSA MCT O/W Pickering 5−50% (w/w) 0.05–5% (w/w) 18,000 rpm for 4 min 10 to 100 μm (Ye et al., 2017)
emulsion
Starch Quinoa seed OSA Lutein in Corn oil Pickering 10–90%, v/v 4% (w/v) 20,000 rpm for 2 min 25.6–43.9 μm (Li et al., 2020)
emulsion gel
Pectin Sugar beet Not mention Limonene oil O/W emulsion 13% (w/v) 2% (w/w) 24,000 rpm for 4 min Not mention (Siew & Williams,
2008a)
Pectin Sugar beet Enzymatic modification Middle-chain O/W emulsion 15% (w/w) 1.5% (w/w) pH 3, 3 μm (Funami et al.,
triglyceride 24,000 rpm for 1 min 2007)
Pectin Sugar beet Enzymatic modification MCT O/W emulsion 15% (w/w) 1% (w/w) pH 3, 24,000 rpm for 3 0.409 to 4.142 (Chen et al., 2016)
min μm
Pectin Sugar beet pulp Different Extraction Soybean oil O/W emulsion 10% (w/w) 1% (w/v) room temperature, 1.12 to 4.12 (Chen et al., 2018)

5
conditions 19,000 rpm for 3 min μm
Pectin Sugar beet Not mention Lactobacillus salivarius S/O/W 10−25% (v/v) 1−4% (w/v) pH 3.9, 12,000 rpm for 7.32 to 16.73 (Zhang et al.,
NRRL 13-30514 in emulsions 4 min μm 2016)
soybean oil
Cellulose nanocrystals Cotton H2SO4 hydrolysis Hexadecane Gel-like o/w 10−86.5% (v/ Not mention ultrasonic 4 μm (Capron & Cathala,
HIPEs v) 2013)
Microcrystalline cellulose (MCC) Cellulose powder Acid hydrolysis and Alkenyl Sunflower oil O/W Pickering 20% (v/v) 0.1−0.2% (w/w) pH 2−8, 10,000 rpm 5 to 15 μm (Kargar et al.,
and modified starch (MS) and waxy maize succinic anhydride emulsion for 7 min 2012)
Gum Arabic Not mention Arabinogalactan protein MCT O/W emulsions 9−14% (v/v) 2−10% (v/v) pH 4, 26,000 rpm for 3 1 μm (Han, Gu et al.,
(AGP) min 2019)
Gum Arabic Not mention Trace elements MCT O/W emulsions 5% (w/w) 5% (w/w) 25 °C, 26,000 rpm for 0.41 μm (Hu et al., 2019)
3 min
Brea gum Not mention Not mention Corn oil O/W emulsions 10% (w/w) 5−20% (w/w) 25 °C, 5000 rpm for 5 783.8 nm (Castel et al.,
min 2017)
Asafoetida gum Oleo-gum-resin of Not mention Rapeseed oil O/W emulsions Not mention 0.5% and 1% (w/v) 20 °C Not mention (Saeidy et al.,
Ferula assa foetida 2018)
root
Inulin Chicory β-lactoglobulin Sunflower oil O/W emulsions 5% (w/w) 2.5−10% (w/w) ＜35 °C, 3500 rpm for 2 to 20 μm (Lopez-Castejon
3 min et al., 2019)
Inulin Not mention OSA and DDSA MCT gold oil O/W emulsions 15% (w/w) 2.5% (w/w) 37 °C 3 to 15 μm (Kokubun et al.,
2018)
Insoluble soybean Defatted soy flour Not mention Refined sunflower oil O/W emulsions 30% (w/w) 1.0–2.0% (w/w) room temperature, 8.0–10.1 μm (Porfiri et al.,
polysaccharides 25,000 rpm for 2 min 2017)
Soybean soluble polysaccharide Not mention Phosphate cross-linked Acidified milk drinks O/W emulsions Not mention 0.05–0.3% (w/w) pH 3.6−4.6 0.5 μm (Nakamura et al.,
2012)
Carbohydrate Polymers 242 (2020) 116388
R. Zhang, et al.
Van Loey, & Hendrickx, 2015; Siew & Williams, 2008a,2008b). The
ideal pectin structure for excellent interface activities, efficient emul-
sification capacity and emulsification stability should contain 3% pro-
tein and a minimum 10% degree of acetylation (Alba & Kontogiorgos,
2017). Also, the molecular weight of pectin should be 100–200 × 103
g/mol and the content of RG-I and ferulic acid should be high (Alba &
Kontogiorgos, 2017). It has been identified that proteinaceous moiety
played an important role in improving the emulsifying properties of
sugar beet pectin (SBP). Loss of the proteinaceous moiety lowered ac-
cessibility of polysaccharide to the emulsion droplets (Funami et al.,
2007). Siew et al. investigated the emulsification ability of SBP to sta-
bilize limonene O/W emulsions and found that both protein and ferulic
acid were adsorbed onto the oil-water interface to stabilize the emul-
sions (Siew & Williams, 2008a,2008b).
Compared with other pectins, SBP possesses worse gelling proper-
ties and better emulsifying properties because of its highly branched
polysaccharide structures, acetyl groups, and protein moiety (Zhang
et al., 2015). Different functional group of SBP can affect its emulsifying
properties (Chen, Fu, & Luo, 2016). Moreover, under different condi-
tions, the functional components including ferulic acid and protein
contents changed greatly, thus affected the emulsifying properties of
pectin. SBP with higher contents of protein and ferulic acid could ad-
sorb favorably to the surface of oil droplets (Chen, Qiu, Liu, Zhu, & Yin,
2018). Elegant studies by Zhang et al. proposed a SBP based solid/oil/
water (SOW) emulsion for spray-dried Lactobacillus salivarius en-
capsulation. Owing to the excellent emulsification property of SBP, the
emulsion based method had higher encapsulation efficiency (up to
87%) and smaller droplets size (less than 17 μm) compared to tradi-
tional methods. The calcium cross-linking SBP could strengthen the
interfacial layer structure, improve the stability of oil droplets and in-
crease cell viability after in vitro digestion (Zhang, Lin, & Zhong, 2016).
2.3. Cellulose derivatives
Cellulose is one of the most abundant, biodegradable and renewable
biopolymer, which can be easily isolated from plants, biomass and
bacteria. It is a linear homopolymer composed of glucose units linked
by β-(1-4) glycosidic bonds. In order to increase hydrophilic nature,
cellulose is prior modified with different functional groups. In most
cases, cellulose could be modified with functional groups at the free
hydroxyls of backbone. For instance, hydroxypropylmethyl cellulose
(HPMC) had methyl groups (hydrophobic) and hydroxypropyl groups
(hydrophilic) along the cellulose backbone thus could act as emulsifier
and adsorb at the oil-water interface (Camino, Perez, Sanchez, Patino, &
Pilosof, 2009). The most common cellulose derivatives include methyl
cellulose (MC), carboxymethyl cellulose (CMC) and HPMC. Both HPMC
and MC were even more surface active than β-lactoglobulin and β-
casein, and both of them could dominate the interfacial properties at
high concentration in the presence of protein (Arboleya & Wilde, 2005).
A MC and HPMC based novel emulsion was designed to replace 75% of
the cream in dairy desserts, which could greatly reduce their fat content
without influencing their organoleptic and textural properties. Different
from the compact and dense microstructure of MC stabilized emulsion,
HPMC stabilized emulsion had a lighter structure and less firmness and
stiffness, which was described sensorially as being smooth and soft
(Borreani, Hernando, Salvador, & Quiles, 2017).
Cellulose particles have been widely applied in stabilizing Pickering
emulsion because of their amphiphilic surface nature from the hydro-
philic edge and hydrophobic face of cellulose chains (Fujisawa,
Togawa, & Kuroda, 2017). Moreover, the packing density of cellulose
particles at the surface of oil droplet could be regulated through tuning
pH and ionic strength (Li et al., 2018). Rod-like cellulose nanocrystals
(CNCs) have been used for stabilizing high internal phase emulsions
(HIPEs) through two-step process (Capron & Cathala, 2013). Rod-like
CNCs were fixed at the oil/water interface along their length, allowing
diff ;usion and reorganization when the volume of the internal phase
6
Carbohydrate Polymers 242 (2020) 116388
increased. As a result, rod-like CNCs could irreversibly adsorb at the
surface of oil droplet and the emulsion with more than 90% hydro-
phobic phase could be stabilized even by less than 0.1% (w/w) of CNCs.
Compared to modified starch particles, cellulose particles could more
efficiently stabilize O/W emulsions and reduce the lipid oxidation rate
due to thicker interfacial layers and negative charge for scavenging free
radicals. Hence, cellulose particles based Pickering emulsion was an
effective means to slow down lipid oxidation (Kargar, Fayazmanesh,
Alavi, Spyropoulos, & Norton, 2012).
2.4. Gum Arabic
GA is an exudate from the Acacia tree species. It is a complex
polysaccharide and the backbone consists of 1,3-linked β-D-galacto-
pyranosyl units. Through hydrophobic interaction chromatography, it
can be separated into three main components including arabinoga-
lactan-peptide (AGp), arabinogalactan-protein (AGP) and glycoproteins
(GP) (Randall, Phillips, & Williams, 1989). AGP has a coiled structure
and can penetrate oil phase at multi-sites, thus provide a perfect an-
choring to the interface (Han, Gu et al., 2019; Han, Hu et al., 2019). The
content of AGP was closely related to the interfacial properties of GA,
and higher AGP content showed better emulsifying capacity to some
extent (Sanchez et al., 2018). When the AGP content increased from 11
to 28%, emulsions exhibited smaller droplet sizes and better stability,
however, when the AGP content further increased to 41%, the droplets
became larger without decreasing the emulsion stability (Han, Gu et al.,
2019; Han, Hu et al., 2019). Moreover, the choice of raw material such
as Acacia species, age of trees and growing conditions play important
roles in the functional properties of GA (Buffo, Reineccius, & Oehlert,
2001). Recently, Hu et al. found that GA rich in trace elements (GARTE)
had a higher AGP content and molecular weight, thus exhibited a better
emulsion stability performance compared to the natural GA. They
proposed that this was attributed to trace elements which could in-
crease surface energy and lead to protein aggregation (Hu et al., 2019).
Despite the excellent emulsifying properties of GA, its high price
and variable supply limited its wider uses and thus studies were con-
ducted to find other similar emulsifiers to replace GA. In that event,
Castel and his/her coworkers found that Brea gum could replace GA to
some extent, as Brea gum stabilized corn oil emulsions exhibited higher
viscosity and stability (Castel, Rubiolo, & Carrara, 2017). Compared to
GA, Brea gum has higher protein content. The polysaccharide-protein
complex in Brea gum gives it high interfacial activity and excellent
emulsifying properties (Castel et al., 2016). In another study (Saeidy
et al., 2018), the monosaccharide composition of asafoetida gum from
Ferula assa-foetida root was similar to GA, however its emulsion stabi-
lity, emulsion capacity and foaming properties were much higher than
GA because of the higher protein content. Wei et al. prepared peach
gum and found that it could enhance the stability of whey protein O/W
emulsions and exhibited no phase separation even after 5 weeks (Wei
et al., 2019).
2.5. Other polysaccharides
Other than the above mentioned polysaccharides, which have been
widely applied for emulsion preparations, chitosan, inulin, soybean
polysaccharides and seaweed polysaccharide have also been used to
stabilize emulsions. Chitosan is an amino polysaccharide consisted of β-
(1,4)-2-acetamino-2-deoxy-D-glucose binary linear units, and has a poor
water solubility because of its rigid crystalline structure. In contrast to
other charged polysaccharides, chitosan is positively charged and can
be incorporated with anionic species such as anionic lipids (Dammak &
Sobral, 2018) to form nanostructures to delivery various bioactive
components. In acidic media, hydrophobic sites and positively charged
amino chitosan groups make chitosan an amphiphilic compound ad-
sorbed readily at the surface of oil droplet through steric and electro-
static effect without any additional surfactant (Schulz, Rodriguez, Del
R. Zhang, et al.
Blanco, Pistonesi, & Agullo, 1998). Higher number and acetyl content of
hydrophobic acetyl groups could improve the emulsion stability of
chitosan (Li & Xia, 2011). Meanwhile, chitosan with the molecular
weight of 410 kDa and 600 kDa had superior emulsifying activity in
their experimental range.
Inulin is a natural fructose polymer linked by β-(1–2)-D-fructosyl-
fructose units, usually contains 2–60 monomers and terminates with a
glucose residue. The degree of polymerization had an important impact
on the physical and chemical properties of inulin. Inulin which had a
high degree of polymerization exhibited poor solubility and high visc-
osity (Lopes et al., 2015). Although no significant surface activity has
been confirmed, inulin still has been widely used in O/W emulsions
because of its potential thickening effect. Thickening of the aqueous
solution can inhibit the destabilization processes such as flocculation
and coalescence to keep the emulsion stable (Lopez-Castejon,
Bengoechea, Espinosa, & Carrera, 2019). In addition, inulin can be
modified with hydrophobical groups to form micellar aggregates for
encapsulating water insoluble bioactive substance. Kokubun and his/
her coworkers synthesized succinylated derivatives of inulin, which
could form micellar aggregates and dissolve hydrophobic compounds.
The succinylated derivatives of inulin could effectively reduce the in-
terfacial tension at the oil-water interface and stabilize O/W emulsions,
has been successfully applied to encapsulate and controlled release of β-
carotene (Kokubun, Ratcliffe, & Williams, 2018).
According to the water solubility of polysaccharides from co-pro-
ducts of soy protein isolation processes, soybean polysaccharides can be
divided into soybean soluble polysaccharides (SSPS) and insoluble
soybean polysaccharides (ISPS). It has been demonstrated that ISPS
could effectively formulate and stabilize acidic and neutral O/W
emulsions after alcoholic treatment of alkaline-insoluble residue, which
could expose internal sites of protein and polysaccharide to increase
their superficial hydrophobicity, thus greatly increased added value of
by-product in soybean industry (Porfiri et al., 2017). In another study, a
SSPS cross-linked high-molecular-mass complex was applied for pre-
paring acidified milk drinks, which showed low viscosity, small particle
size, and could keep stable for 14 days (Nakamura, Fujii, Tobe, Adachi,
& Hirotsuka, 2012).
Seaweed is an important natural source of polysaccharide, which
contains lots of cell wall polysaccharides, mycopolysaccharides and
storage polysaccharides. Alginate is a linear anionic polysaccharide
originated from brown seaweed, mainly composed of mannuronic acid
and guluronic acid units. Another seaweed polysaccharide carrageenan
is a kind of sulphated polygalactan derived from red seaweed. Melanie
and his/her coworkers prepared DSA-modified alginate and carra-
geenan, and evaluated their rheological and emulsifying properties
respectively. With the increase concentration of DSA-modified seaweed
polysaccharides, the droplet size became smaller. The results showed
that DSA-modified seaweed polysaccharides could greatly decrease the
interfacial tension at the interface and exhibited excellent emulsifica-
tion performance (Melanie et al., 2020).
3. Polysaccharides based complexes as emulsifiers
Although polysaccharides alone exhibit certain emulsification
ability, in most cases, polysaccharides usually play roles together with
other emulsifiers to simultaneously improve the stability of emulsions.
Complexes of emulsifying biopolymers based on polysaccharide-poly-
saccharide interaction, polysaccharide-surfactant interaction or poly-
saccharide-protein interaction have been used as efficient emulsifiers to
produce stable O/W emulsions. As shown in Fig. 4, the complexes can
be formed through covalent bond and non-covalent bond (electrostatic
interaction, hydrophobic interaction and hydrogen bond). Covalent
bond is specific, strong and irreversible while non-covalent interaction
is much weaker and can be broken under certain conditions. Table 2
summarized several polysaccharide complex stabilized emulsions for
encapsulation and delivery of bioactive food ingredients.
7
Carbohydrate Polymers 242 (2020) 116388
3.1. Polysaccharides-polysaccharides stabilized emulsions
Multiple polysaccharides have synergistic effect when applied to
stabilize emulsions. For instance, different concentrations and ratios of
GA and Dioscorea opposita polysaccharides (DOP) had different effects
on the droplet sizes and stabilities of emulsions (Ma et al., 2017). When
the ratios of MCT, GA and DOP were kept up to 1:1:1, the poly-
saccharide complex showed best emulsifying performance, and could
be better used to encapsulate bioactive food ingredients. Similarly,
when applied apricot gum (AG) as first emulsifier and apple pectin as
second emulsifier for stabilizing O/W emulsion, the ratio of AG/pectin
had an obvious effect on the size of droplet, Zeta potential and stability
of emulsions because high AG content could suppress small eddies
formation during homogenization and increase negative surface charge
of droplets (Shamsara, Jafari, & Muhidinov, 2017). Trujillo-Cayado and
his/her coworkers studied the influence of different concentrations and
ratios of two microbial polysaccharides on the rheological properties of
α-pinene/water emulsions. They found that the lower gum concentra-
tions led to oil droplets with smaller Sauter mean diameter, and the
dynamic viscoelastic properties of emulsion were significantly influ-
enced by rhamsan/welan mass ratio (Trujillo-Cayado, Alfaro, Munoz,
Raymundo, & Sousa, 2016). He et al. combined OSA modified starch
with xanthan gum (XG) to form complex carrier to encapsulate con-
jugated linoleic acid (CLA). They confirmed that the OSA starch-XG
nanoparticles showed greater emulsion stability than OSA starch na-
noparticles without XG. OSA starch was performed as the main wall
material to deliver CLA, and further XG could stabilize and improve the
performance of the carrier, both of them provided good protection for
CLA against oxidation (He et al., 2016).
HIPE is defined as a unique emulsion system whose internal phase
volume fraction is more than 0.74. Its structure is similar to the tradi-
tional low liquid content gas-liquid foam, and thus exhibit unique and
fascinating performance, such as high viscosity and viscoelastic rheo-
logical behavior (Cameron & Sherrington, 1996). Cationic chitosan
could interact with other anionic polysaccharides through electrostatic
interaction to form HIPE. As shown in Fig. 5A, a chitosan and OSA
starch based electrostatic polysaccharide complex to prepare a HIPE
was constructed (Yan et al., 2019). The positively charged chitosan
could enhance the wettability of OSA starch, and the formed OSA
starch/chitosan complex could promote the formation of HIPE with a
stable gel-like structure. The complex formed a robust shell around the
droplet and acted as a barrier to hinder the contact between pro-oxidant
and oil. Similarly, Tan and his/her coworkers proposed a simple
synthesis of renewable HIPEs based on successive cross-linking and
electrostatics of chitosan and pectin without any surfactants, synthetic
polymers or colloidal particles. The morphology, rheology and pro-
cessability of HIPE could be nicely controlled by changing ultrasonic
intensity and polysaccharide ionization. The ultrasonic processing
could produce cross-linked polysaccharide shells on the surface of
droplets through acoustic cavitation and emulsifying effects, which
played important roles in inhibiting phase separation and enabling
stable HIPEs formation (Tan, Pajoumshariati, Arshadi, & Abbaspourrad,
2019) (Fig. 5B).
3.2. Surfactant-polysaccharides stabilized emulsions
The presence of surfactant in polysaccharide stabilized emulsions
can significantly affect the composition and structure of the adsorption
layers and rheological properties (Duner, Kim, Tilton, Garoff, &
Przybycien, 2016). Surfactants can prevent droplet coalescence by ad-
sorbing at the surface of droplet and increasing their repulsive inter-
actions, thus provide long-term stability to emulsions. The interactions
between surfactants and polysaccharides depend on the nature of the
surfactant, chemical composition of polysaccharide chain and electrical
charges involved. For instance, quaternized chitosan and sodium 1-
decanesulfonate could form complex through strong electrostatic
R. Zhang, et al.
Fig. 4. Schematic presentation of covalent and non-covalent interaction (electrostatic interaction, hydrophobic interaction and hydrogen bond) in polysaccharides
based complexes.
interaction, and the degree of surfactant-polysaccharides association
was up to 0.74 (Senra et al., 2018). The complex exhibited better in-
terfacial properties than quaternized chitosan or surfactant alone, and
could increase viscoelastic moduli of the interfacial layer.
Non-ionic surfactants as emulsifiers are not influenced by the ionic
strength and they can promote a steric stabilization mechanism in
emulsions. The size and architecture of polysaccharide/surfactant
complex are dependent on the concentration and structure of the sur-
factant employed. Small variations in surfactants structure could result
in significant differences in intermolecular interactions and association
with polysaccharides (Grant, Lee, Liu, & Allen, 2008). When mixing
natural cationic polysaccharide chitosan with three kinds of nonionic
surfactants including sorbitan monolaurate, sorbitan monooleate and
sorbitan triooleate respectively, the degree of saturation, length of the
surfactant hydrocarbon chains and chemical architecture had important
impacts on the development of chitosan–surfactant system (Grant, Cho,
& Allen, 2006). Trujillo-Cayado and his/her coworkers applied non-
ionic surfactant (polyoxyethylene glycerol esters) and polysaccharides
(rhamsan gum and welan gum) to O/W emulsion and studied its small
amplitude oscillatory shear and steady shear flow properties. The re-
sults of mechanical spectra and flow curves exhibited the filler role of
the surfactant and the blends of rhamsan/welan gave intermediate
viscoelasticity and low shear viscosities (Trujillo-Cayado, Alfaro,
Raymundo, Sousa, & Munoz, 2016).
3.3. Protein-polysaccharides stabilized emulsions
Emulsions stabilized by protein-polysaccharide complexes show
more resistance to environmental stresses than those stabilized by
protein alone (Pereira, Cattelan, & Nicoletti, 2019). High molecular
weight polysaccharide protein complex could greatly improve their
overall solubility in emulsion with consequent improvements for
8
Carbohydrate Polymers 242 (2020) 116388
emulsification properties (Li, Xiang, Wang, & Gong, 2019). For in-
stance, combination casein with OSA starch through hydrogen-bonding
interaction could greatly improve the nanoemulsion stability to en-
vironment stresses (Yang, Qin, Kan, Liu, & Zhong, 2019). The sodium
caseinate stabilized emulsion was unstable when close to its isoelectric
point and the droplets tended to aggregate under acidic conditions. The
addition of λ-carrageenan could increase aqueous phase viscosity and
electrostatic repulsion between the droplets, thus improved the emul-
sion stability at low pH (Koo et al., 2019). In the protein-poly-
saccharides stabilized emulsion, proteins had surface-active properties
and could adsorb at oil/water interface through electrostatic and steric
mechanisms, meanwhile polysaccharides had water-binding, gelling
and thickening properties, and could inhibit droplet movement. How-
ever, in some situations, polysaccharides could dominate the interface.
For instance, when competitive adsorption of soy protein and HPMC, it
was HPMC that controlled the emulsions size and dominated the in-
terface (Bellesi, Ruiz-Henestrosa, & Pilosof, 2020).
Interactions between polysaccharides and proteins include non-
covalent interaction and covalent interaction. Physical mixing of pro-
teins and polysaccharides could lead to non-covalent interactions such
as electrostatic interaction, hydrophobic interaction and hydrogen
bond, which were non-specific and unstable, and could be affected by
pH, ionic strength, temperature, concentration and so on. Among them,
it was obvious that pH was the major determinant of interaction be-
tween protein and polysaccharide. For instance, pH had a great influ-
ence on the interaction between soy protein isolated (SPI) and soy hull
polysaccharides (SPH). At pH 2.0–4.0, the SPH adsorbed at the surface
of SPI to neutralize the positive charged SPI. When the pH increased
from 5 to 9, the mean volume diameter of oil droplets decreased and the
interaction between biopolymers and oil molecules increased (Wang,
Luo et al., 2020; Wang, Yang et al., 2020). Protein polysaccharide
covalent conjugation could be realized through enzymatic conjugation
 R. Zhang, et al.

Table 2
Summarization of polysaccharide complex stabilized emulsions for encapsulation and delivery of bioactive food ingredients.
Polysaccharide Substance Polysaccharide Interaction Oil phase Type of emulsion Ratio of oil phase Preparation conditions Droplet size References
/substance ratio

Gum Arabic Dioscorea opposita 1−3.5 (w/w) Not mention MCT O/W emulsions 20−70% (v/v) 20 °C, pH 7.0 0.16 to 0.28 (Ma et al., 2017)
polysaccharides μm
Apricot gum Apple pectin 7.13−35.6 (w/w) Not mention Sunflower oil O/W nano-emulsions 25% (v/v) 30 °C, pH 2−7, 15,000 350 to 700 (Shamsara et al.,
rpm for 20 min nm 2017)
Rhamsan gum Welan gum 0−1 (w/w) Not mention α-pinene O/W emulsions 30% (w/v) room temperature, 300 0.5 to 3 μm (Trujillo-Cayado,
rpm for 30 min Alfaro, Munoz et al.,
2016)
OSA starch Chitosan 2.5−20 (w/w) Electrostatic DHA-rich algae oil High Internal Phase 75% (w/w) 12,000 rpm for 3 min 0.1–5 μm (Yan et al., 2019)
interaction Emulsion
Chitosan Pectin 1 (w/w) Cross-link functional Corn oil Renewable high 79.4−89.8% (v/ 13,000 rpm 1 μm (Tan et al., 2019)
groups internal phase v)
emulsions
Chitosan Sodium 1- 1 (v/v) Electrostatic Sunflower oil O/W emulsions 25% (w/w) 7500 rpm for 3 min Not (Senra et al., 2018)
decanesulfonate interaction mention
Rhamsan gum and welan Polyoxyethylene glycerol 0.3:0.3:3.5 to Hydrophilic- Coconut oil O/W emulsions 30% (w/w) 20 °C, 9500 rpm for 2 Not (Trujillo-Cayado,
gum ester 0.8:0.8:3.5 (w/w) lipophilic balance min mention Alfaro, Munoz et al.,

9
number 2016)
OSA Casein 0.25 (w/w) Hydrogen-bonding Fish oil O/W emulsions 1% (w/w) 20 °C, 20,000 rpm for 3 236 nm (Yang et al., 2019)
interaction min
Carrageenan Sodium caseinate and 1:50:50 to 35:50:50 w/ Not mention MCT O/W emulsions 10% (v/v) 25 °C, pH 7 12,000 0.1 to 1 μm (Koo et al., 2019)
soy lecithin w rpm for 1min
HPMC Soy protein 0.5 (w/w) Not mention Sunflower oil O/W emulsions 10% (v/v) < 25 °C, ultrasonic 0.3 to 2 μm (Bellesi et al., 2020)
Soy hull polysaccharides Soy protein isolated 2.5 (w/w) Electrostatic Soy oil O/W emulsions 10% (w/w) pH 2−9, 10, 8 to 80 μm (Wang, Luo et al.,
interaction 000 r/min for 2 min 2020)
Pectin and gum Arabic Sodium casemate 1:1:2 (w/w) Electrostatic α-tocopherol and O/W emulsions 5% (w/w) 10 °C, 10,000 rpm for 300 and (Cheng et al., 2020)
interaction resveratrol in 1min 860 nm
sunflower oil
Anionic polysaccharides Lentil protein isolate 0.25 (w/w) electrostatic Canola oil O/W emulsions 50% (w/w) pH 2.6−4.0, 7200 rpm 5 to 337 μm (Wang, Nian et al.,
interaction for 5min 2019)
Six kinds of Lysozyme amyloid fibrils 1 (v/v) Electrostatic β-carotene in high internal phase ＞74% (v/v) 10,000 rpm for 2 min 100 μm (Wang, Nian et al.,
polysaccharides interaction dodecane emulsions 2019)
Chitosan Gliadin 0.02 (w/w) Not mention Curcumin in Corn oil Pickering high 50−90% (v/v) room temperature, 20 to 100 (Zeng et al., 2017)
internal phase 20,000 rpm for 2 min μm
emulsions
Gum acacia Whey protein isolate 2 (w/w) Maillard reaction Soybean oil O/W emulsions 25% (v/v) room temperature, Not (Chen et al., 2019)
Covalent bonding 13,500 rpm for 2 min mention
Gum Arabic Pea protein isolate 4 (w/w) Maillard reaction Corn oil O/W emulsions 2% (w/w) 0 °C, pH 7 0.5 μm (Zha et al., 2019)
Covalent bonding
Lotus root amylopectin Whey protein isolate 1 (w/w) Covalent bonding Soybean oil O/W emulsions 50% (v/v) 10,000 rpm for 1 min 1 μm (Bai et al., 2019)
Carbohydrate Polymers 242 (2020) 116388
R. Zhang, et al.
Fig. 5. Microstructure of HIPEs. (A) Chitosan and OSA starch stabilized HIPEs (Yan et al., 2019). (B) Chitosan and pectin stabilized HIPEs (Tan et al., 2019).
(Matalanis & McClements, 2012), chemical cross-linking (Chao, Taoran,
Qiaobin, & Yangchao, 2017) and Maillard reaction (Nooshkam &
Varidi, 2020).
The emulsifying capacity of protein-polysaccharide complex is as-
sociated with the type of polysaccharides. For instance, resveratrol was
vulnerable to degradation and oxidation, with the percentage dropping
by 90% after 7 days in phosphate buffer (Zupancic, Lavric, & Kristl,
2015). When encapsulated resveratrol in O/W emulsions stabilized by
sodium caseinate (SC)-pectin complex or SC-GA complex, the size, Zeta
potential and surface coverage of oil droplets increased compared to the
emulsions stabilized by SC alone (Cheng, Fan, Liu, Wusigale, & Liang,
2020). Both GA and pectin could increase accumulation and stability of
resveratrol, and pectin exhibited better performance than GA because
pectin could induce higher bulk viscosity at the same polysaccharide
concentration. The results showed that the protected resveratrol in
emulsions degraded slightly with a percentage of about 76% remaining
after storage for 42 days. Wang et al. compared the emulsifying prop-
erties of four complex composed of lentil protein isolate (LPI) with four
different polysaccharides (CMC, GA, alginate (AL), and ι-carrageenan
(CAR)). The formed LPI-CAR complex was much smaller than other
complexes in solution because of the large electrostatic repulsive forces
exerted between CAR chains. They found that the LPI-CAR stabilized
emulsion exhibited higher stability because of the smaller droplet sizes,
higher continuous phase and emulsion viscosity, and stronger electro-
static repulsion between negatively charged droplets, thus confirmed
their hypothesis that smaller LPI-polysaccharide complexes could be
better emulsifiers because of their better ability to migrate and orient at
the surface of oil droplets (Wang, Nian et al., 2019; Wang, Ghosh et al.,
2019).
Protein-polysaccharides complex could also be applied to stabilize
HIPEs. Different from the precipitated coacervates of polysaccharides
and globule protein monomers, polysaccharides and amyloid fibrils
10
Carbohydrate Polymers 242 (2020) 116388
could form well dispersed coacervates and exhibit better ability to
stabilize HIPEs because of the enhanced modulus of the disperse phase
and the filler-like effect among the oil droplets. Under the protection of
the interfacial amyloid fibrils-polysaccharides complex, the en-
capsulated β-carotene could keep stable after thermal treatment, ul-
traviolet irradiation and iron ions in aqueous phase (Wang, Nian et al.,
2019; Wang, Ghosh et al., 2019). A facile anti-solvent method was
applied to fabricate gliadin/chitosan hybrid particles (GCHPs) (Zeng
et al., 2017). The prepared GCHPs were able to effectively adsorb and
anchor at the surface of oil droplet to steric hindrance against the
coalescence. Hence, GCHPs could stabilize Pickering HIPEs with in-
ternal phases up to 83% at a very low particle concentration (0.5–2%).
Moreover, the formed Pickering HIPEs could effectively retard primary
lipid oxidation and protect the chemical stability of the encapsulated
curcumin against UV radiation. Wei and his/her coworkers prepared a
high internal phase Pickering emulsions stabilized by ovo-
transferrin–GA particles (OVT–GA particles) for curcumin delivery
dissolved in MCT oil. The rheological properties and oil droplet size of
HIPEs depended on both oil fraction and particle concentration.
Moreover, the OVT–GA particles based Pickering emulsion could not
only increase the extent of lipolysis but also improve the bioaccessi-
bility of loaded curcumin because the OVT–GA particles were easily
dissociated in the gastrointestinal tract to facilitate release of curcumin
(Wei & Huang, 2019).
Whey protein isolate (WPI) has been widely applied in foods and
beverages as natural emulsifier. However, WPI stabilized emulsions are
sensitive to ionic strength, pH and thermal treatment. Lots of studies
have focused on the covalent interaction between polysaccharides and
WPI to effectively enhance the emulsifying properties of WPI.
Conjugated lotus root amylopectin (LRA) to WPI through dry-heat re-
action could form WPI-LRA complex, which exhibited good emulsifying
ability and storage stability. However, it was still unstable and could be
R. Zhang, et al.
influenced by pH and NaCl concentration to some extent (Bai et al.,
2019). When conjugated WPI to gum acacia (GA) via the Maillard re-
action, the functionality of WPI under conditions of different pH, ionic
strength, and temperature was improved because hydrophilic GA im-
proved the affinity of WPI to water molecules and limited the interac-
tion between WPI under unfavorable conditions (Chen et al., 2019).
The results showed that the Maillard reaction significantly decreased
the surface hydrophobicity and fluorescent intensity of WPI, and the
generated conjugates exhibited improved solubility, stability and
emulsion properties. Maillard reaction with hydrophilic poly-
saccharides was a practical way to improve the solubility and func-
tionality of poor water soluble proteins. Another study also applied
Maillard reaction to conjugate Pea protein isolate and GA. The con-
jugate enhanced protein solubility, improved physical stability and
anti-oxidation of corn oil-in-water emulsions (Zha, Dong, Rao, & Chen,
2019).
4. Bioavailability of polysaccharides based delivery systems: in
vitro and in vivo models
The low absorption and bioavailability of bioactive food compo-
nents are attributed to both environmental conditions (heat, pH, light,
oxygen) and physiological conditions (pH, enzymes, intestinal mucus
barrier). One of the most important parameters for characterizing the
effectiveness of an emulsion delivery system is that the encapsulated
components are protected until reached to the targeted location. Hence,
in vitro and in vivo models have been applied to assess the absorption
and bioavailability of bioactive components loaded in the emulsions
(Fig. 6). Table 3 summarized several in vitro and in vivo models to study
digestion of polysaccharide stabilized emulsions.
4.1. In vitro models
In vitro evaluation of digestion of encapsulated bioactive food in-
gredients in emulsion delivery system usually includes three stages
namely simulated oral, gastric and intestinal phase. As shown in Fig. 6,
an initial simulated oral stage contains α-amylase, mucin and a nearly
neutral pH value at the temperature of 37 °C for about five minutes.
Simulated gastric fluids includes salts, acids, pepsin, lipase and an
Fig. 6. In vitro and in vivo models to simulate digestion of emulsions.
11
Carbohydrate Polymers 242 (2020) 116388
extremely low pH value at the temperature of 37 °C for about two
hours. Simulated intestinal fluids includes bile salts, a series of digestive
enzymes (such as trypsin, amylase, lipase), salts (NaCl or CaCl2) at the
pH values around 6.5–7.5 for about three hours at a body temperature
of 37 °C. The in vitro simulated gastrointestinal tract model has been
widely applied in the area of functional food due to its advantages of
cheap, time-saving and highly reproducible, thus became an excellent
alternative to animal or human experiments.
In recent years, many researchers have been focused on studying the
relationship between interface composition and lipid digestion in food
O/W emulsions. Polysaccharide based O/W emulsions could be applied
to increase the absorption and bioavailability of loaded hydrophobic
components or exploited to slow down lipolysis to reduce calorie in-
take. A large number of studies have reported that polysaccharides,
including chitosan, pectin, carrageenan, starch, alginate, and methyl
cellulose, would have a potential influence on the gastrointestinal fate
of edible food emulsions (Chang & McClements, 2016). The char-
acteristics of the interfacial layers on the surface of oil droplets were of
great importance to the lipid digestion extent and release rate of en-
trapped components. The lipid digestion process firstly takes place in
stomach but 70–90% of the fat digestion was in small intestine by
pancreatic lipase in humans (Bauer, Jakob, & Mosenthin, 2005). During
the process of digestion, the emulsion went through the physical and
biochemical environment changes and led to flocculation, coalescence,
aggregation and droplet disruption (Fig. 6). Commonly, the size of
droplet increased after mouth-stomach digestion stage and disrupted
after intestinal digestion stage (Fig. 6). For instance, in Ulva fasciata
polysaccharide (UFP) stabilized O/W emulsions loaded with β-car-
otene, the oil droplet size increased from 1.91 μm to 2.86 μm after
mouth-stomach digestion stage, which was attributed to the depletion
and bridging flocculation of the lipid droplets by mucin. After intestinal
digestion stage, the size decreased obviously attributed to the catalysis
by cholate and pancreatic enzymes (Shao, Qiu, Xiao, Zhu, & Sun, 2017).
Different kinds of polysaccharides varied in their abilities to stabi-
lize emulsions under gastrointestinal conditions because of the differ-
ence in surface charge and hydrophobicity (Costa et al., 2020). Fur-
thermore, same kind of polysaccharide from different sources also
exhibited different effects on lipid digestion process. For instance,
pectic polysaccharides from different apples and citruses showed
R. Zhang, et al. Carbohydrate Polymers 242 (2020) 116388

different effects on the digestion of emulsified lipids and activities of

(Aguilera-Angel et al., 2018)

(Cervantes-Paz et al., 2016)

(Malinauskyte et al., 2018)

pancreatic lipase due to their difference in molecular weight and

(Vecchione et al., 2016)

methoxylation degree (Aguilera-Angel, Espinal-Ruiz, & Narvaez-

(Wei & Huang, 2019)

(Picone et al., 2017)

(Wang et al., 2016)

(Costa et al., 2020)
Cuenca, 2018). The amount and properties of pectin determined the

(Shao et al., 2017)

(Feng et al., 2017)
process of carotenoid micellarization. Low pectin concentrations tend
to bind bile salt and form carotenoid micellarization, while high pectin
References

concentrations tend to increase the gastrointestinal medium viscosity

and form large particle sizes. Micellarization of free carotenoids was
favored by high DME through bile salts binding capacity while mi-
Compared with bulk MCT oil, ovotransferrin-GA particles stabilized HIPEs improved both extent of lipolysis

Chitosan-stabilized emulsion kept stable after gastric digestion but aggregated obviously after intestinal step

Pectins with high molecular weight and viscosity increased the micellarization of the less polar carotenoids
cellarization of the less polar carotenoids was influenced by high mo-
Increased degree of methoxylation of pectic polysaccharides had better ability to inhibit enzyme activity

Bilayer emulsions could reduce triglyceride level in the blood of rats and had a lower fat bioavailability

The best formulation for high curcumin bioavailability was a combination of a small nanoemulsion size
Cellulose nanofibers-stabilized emulsion showed a slight aggregation after gastric step and was able to
Digested Ulva fasciata polysaccharide stabilized emulsions showed higher lipid digestion rate than GA
Corn fiber gums stabilized emulsion could increase the extent of lipolysis and bioavailability of lutein

lecular weight and viscosity. High degree of methyl esterification fa-

The BSA-dextran stabilized emulsion could increase curcumin oral bioavailability in mice by 4.8-fold
(110 nm), co-delivery of curcumin and piperine (weight ratio 100: 1) and a high degree of chitosan
Pectins with high and medium degree of methyl esterification promoted lipolysis, bile binding and vored micellarization of free carotenoids through great bile salts
binding capacity, high molecular weight and viscosity influenced mi-
cellarization of the less polar carotenoids (Cervantes-Paz et al., 2016).
Probiotics has become one of the most popular health products in
recent years. However, the viability of probiotics was greatly reduced
along the digestive tract. Incorporation probiotics into food matrices
Emulsion gelation improved probiotic resistance to in vitro digestion conditions

through emulsions has emerged as a promising technique to maintain

their viability. Picone and his/her co-workers added gelation to W/O
emulsion to formed emulsion gelation to delivery Lactobacillus rham-
nosus (Picone et al., 2017). Compared to free culture, the survival rate
of Lactobacillus rhamnosus encapsulated in emulsion gelation was in-
creased from 35% to 77% after in vitro digestion. The results showed
stabilized emulsions and beet pectin stabilized emulsions

that rheological properties of the encapsulation matrix had an im-

portant effect on cell viability. The gellan gel network could act as an
compared with curcumin/Tween 20 suspension

extra barrier during gastric digestion, thus were more efficient to pro-
micellarization of the more polar carotenoids.
inhibit lipid digestion in intestinal condition

tect probiotic. Moreover, they found that emulsion gelation was stable
after oral and gastric digestion, and was destabilized by enteric fluid.

4.2. In vivo models

and curcumin bioaccessibility

In vivo models for studying the digestion and absorption of bioactive

thiolation (14−15%)

food ingredients loaded in emulsions have been rare reported because

of the long test period and high cost. However, such studies are of great
significance to understand the physiological effects on the emulsion
Main results
Summarization of in vitro and in vivo models to study digestion of polysaccharide stabilized emulsions.

delivery system, and can provide more information about absorption

and bioavailability of the loaded compounds. For instance, the tissue
distributions of the encapsulated curcumin could be investigated
through in vivo models. The curcumin-loaded O/W emulsion was sta-
internal phase Pickering

bilized by bovine serum protein and dextran conjugate through

Gelation of O/W emulsion

Maillard reaction. The curcumin was mainly distributed in gastro-

O/W Pickering emulsion

O/W bilayer emulsions

intestinal tract of mice after oral administration of about one hour and
O/W nano-emulsions

almost disappeared after 24 h of post-administration, which implied

Type of emulsion

emulsions

O/W emulsions
emulsion

emulsion

O/W emulsion
O/W emulsion

that the formed emulsion could not only inhibit loaded curcumin de-
composition but also promote curcumin absorption in vivo, and was an
excellent oral delivery system for hydrophobic bioactive food in-
O/W

O/W
O/W
High

gredients (Wang, Liu, Xu, Yin, & Yao, 2016).

Control the extent of lipid digestion could be realized by adjusting
β-carotene in soybean

Curcumin in soybean
Curcumin in MCT oil

Curcumin in MCT oil

the composition and structure of emulsion interface layer. Malinauskyte

Lutein in corn oil

et al. studied the impact of interfacial composition of emulsion on lipid

Carotenoids in
Sunflower oil

digestion in rats. The prepared O/W emulsions were stabilized by whey

Encapsulated

Lactobacillus

Rapeseed oil
components

Soybean oil

soybean oil

rhamnosus

proteins and whey proteins-CMC respectively. They measured fat con-

tent in feces and recorded the plasma triglyceride content after oral
oil

oil

administration of the prepared emulsion for two hours. The results

showed that whey proteins-CMC stabilized emulsion had a lower fat
Ulva fasciata polysaccharide

bioavailability and a reduction in the triglyceride level in the blood of

Ovotransferrin-GA particles

rats. Hence, oil droplets surrounded by multilayers had better stability

carboxymethyl cellulose
Thiol modified chitosan
Deacylated gellan gum
Cellulose and Chitosan

Pectic polysaccharides

against environmental stresses compared to conventional monolayer

Whey proteins and

(Malinauskyte et al., 2018).

Corn fiber gums
Polysaccharide

The size distribution of oil droplets could also greatly influence the
BSA-dextran

bioavailability of bioactive component in vivo. First, small droplets can

be digested more quickly by digestive enzymes because of the large
Pectin

surface area. Second, small droplets can penetrate into the mucous
layer to increase their residence time. Third, pretty small droplets could
In vitro
Table 3

In vivo
Model

directly transport across epithelium cell layer through paracellular or

transcellular mechanism (McClements, 2011). For instance, different

12
R. Zhang, et al.
size (110 nm and 230 nm) of oil droplet loaded with curcumin had
different bioavailability in vivo. Smaller droplet size had better bioa-
vailability, and the bioavailability of curcumin loaded in the prepared
110 nm nano-emulsion was 64 times higher than that of unformulated
curcumin (Vecchione et al., 2016).
5. Discussion
Emulsifier is one of the most important food additives in food in-
dustry. The demand for natural, safe and nutritious emulsifiers is in-
creasing (McClements et al., 2017). Compared to synthetic emulsifiers
such as sorbitan esters and sucrose esters, polysaccharide is safer and
can even increase the nutritional and health functions of food (Xing,
Zhang, Hu, Wu, & Xu, 2009). The properties of polysaccharides greatly
depend on their molecular weight, branching degree, composition,
structure and conformation (Kontogiorgos, 2019). Most poly-
saccharides have strong hydrophilicity, low flexibility and simple
monomer repeat backbone, resulting in their surface activities much
lower than that of proteins. When graft with protein groups or hydro-
phobic chemical groups such as acetyl group and methoxy group,
polysaccharides can exhibit great surface activities. For example,
starch, cellulose, inulin and alginate can become surface active after
hydrophobic modifications. For this reason, these polysaccharides are
actually not natural. The most widely used truly natural polysaccharide
emulsifiers include GA, pectin and chitosan. GA is composed of a hy-
drophobic polypeptide backbone and plenty of hydrophilic anionic
polysaccharide chains. Hydrophobic polypeptide backbone can anchor
to the surface of oil droplet, meanwhile hydrophilic anionic poly-
saccharide chains can provide steric and electrostatic stabilization. Si-
milarly, pectins isolated from various plants usually consist of a hy-
drophobic protein or phenolic fraction, and a hydrophilic
polysaccharide fraction. In acidic media, hydrophobic sites and posi-
tively charged amino chitosan groups make chitosan an amphiphilic
compound.
Emulsification is one of the most important properties of amphi-
philic polysaccharides. Moreover, polysaccharides such as starch and
CMC can be used as thickening agents to stabilize emulsions. On the one
hand, the polysaccharide molecules are firmly adsorbed at the oil-water
interface through the affinity between hydrophobic group and oil
phase, forming a protective film on the surface of the oil droplet, re-
ducing the interfacial tension between oil and water, thus preventing
the condensation of oil drop and oil-water stratification. On the other
hand, polysaccharides contain a large number of hydrophilic groups,
which can interact with water molecules and increase viscosity.
Polysaccharides with extended molecular structures have better ability
to stabilize emulsion compared to compact structure because extended
molecular structures can entrain large quantities of water, increase
solution viscosity and promote depletion flocculation (Bai et al., 2017).
Therefore, the stability of emulsion system can be improved by in-
creasing the viscosity of emulsion, reducing the diffusion coefficient of
droplets in the emulsion and decreasing the frequency of collision and
coalescence between droplets (Dickinson, 2003). The thickening effect
depends on the type and concentration of polysaccharides, the pH of the
food system and the temperature. For instance, xanthan can maintain
viscosity in the presence of electrolytes, high temperature and wide pH
ranges (Sahin & Ozdemir, 2004) while CMC will reduce viscosity in the
presence of electrolytes or at low pH (Koocheki, Ghandi, Razavi,
Mortazavi, & Vasiljevic, 2009). The viscosity of emulsion increases with
the increase of molecular mass, electrostatic charge density and chain
rigidity. And linear polysaccharide has higher viscosity compared to
branched polysaccharides (Saha & Bhattacharya, 2010).
Moreover, many studies have showed that polysaccharides could
interfere lipid digestion when applied polysaccharides stabilized
emulsion for delivery of food bioactives (Espinal-Ruiz, Restrepo-
Sanchez, Narvaez-Cuenca, & McClements, 2016; Verrijssen et al.,
2014). Different kinds of polysaccharides may affect the digestion of
13
Carbohydrate Polymers 242 (2020) 116388
emulsified lipids through different mechanisms because of the differ-
ence in surface activities, binding characteristics, thickening, and ge-
lation behavior (Gidley, 2013; Li & Nie, 2016). For instance, cationic
chitosan can bind to bile salt, induce droplet flocculation, increase
viscosity of gastrointestinal fluids to retard the digestion of emulsified
lipids (Qin, Yang, Gao, Yao, & McClements, 2016; Li & McClements,
2014). Anionic alginate can bind to calcium ion and fatty acid, induce
depletion flocculation, modulate rheology of gastrointestinal fluids to
retard the digestion of emulsified lipids (Hu, Li, Decker, & McClements,
2010; Li & McClements, 2011, 2014).
The major advantages of polysaccharides as emulsifiers are that the
produced oil droplets are relatively stable to changes in ionic strength,
pH, or temperature because they can form thick hydrophilic coatings on
the surface of oil droplets (McClements, 2016). Meanwhile, poly-
saccharides can act as thickeners to further stabilize emulsion and po-
tentially influence the gastrointestinal fate of the encapsulated bioac-
tive food ingredients. However, adsorption kinetics showed that most
polysaccharides adsorbed slowly around oil droplet, which can lead to
droplet coalescence during homogenization. In addition, poly-
saccharides had lower ability to reduce interfacial tensions compared to
proteins and small surfactant (Chang, Tu, Ghosh, & Nickerson, 2015;
Huang, Kakuda, & Cui, 2001).
6. Conclusions and future perspectives
In conclusion, the present review comprehensively summarizes the
polysaccharides and their complexes stabilized emulsions for en-
capsulation and delivery of bioactive food ingredients. Both in vitro and
in vivo models proved that polysaccharides stabilized emulsions could
improve their stabilities and bioavailabilities. Polysaccharides are
widely available and have a variety of structures with different ad-
vantages including non-toxic, easily digested, biocompatible and can
keep stable over a wide range of pH and temperatures. In addition, they
can even act as thickeners and weighting agents, which are ideal sta-
bilizers to stabilize emulsions. Reasonable choice of other emulsifiers to
interact with polysaccharides will exhibit synergistic effects to co-sta-
bilize emulsions. Despite the fact that a number of studies have con-
ducted on developing emulsions containing polysaccharides and their
complexes for encapsulating and delivery of bioactive food compo-
nents, some gaps still need to be covered. Thus, we recommend that the
future developments of polysaccharides stabilized emulsions should
focus on the following points, (i) investigation of novel hydrophobic
group to modify polysaccharides to further improve their emulsifying
properties; (ii) development of new food-grade reactions which can be
applied to produce polysaccharides conjugates with novel functional
properties; and (iii) more realistic models should be taken into account
such as mucus barriers, cellular uptake and transportation mechanisms.
Acknowledgements
This work was supported by the Key Research and Development
Program of Zhejiang Province (2020C02037, 2020C02040), China.
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