Recent Advances in Food Emulsions and Engineering Foodstuffs Using Plant-Based Nanocelluloses

FO12CH01_Bai ARjats.
cls November 28, 2020 12:24
Annual Review of Food Science and Technology

Recent Advances in Food
Emulsions and Engineering
Foodstuffs Using Plant-Based
Nanocelluloses
Access provided by Auckland University of Technology on 12/12/20. For personal use only.
Annu. Rev. Food Sci. Technol. 2021.12. Downloaded from www.annualreviews.org
Long Bai,1,2 Siqi Huan,1,2 Ya Zhu,3 Guang Chu,3

David Julian McClements,4 and Orlando J. Rojas2,3
1
Key Laboratory of Bio-Based Material Science and Technology of Ministry of Education,
College of Material Science and Engineering, Northeast Forestry University, Harbin,
Heilongjiang 150040, China; email: longbai2011@hotmail.com
2
Bioproducts Institute, Departments of Chemical and Biological Engineering, Chemistry, and
Wood Science, The University of British Columbia, Vancouver, British Columbia V6T 1Z3,
Canada
3
Bio-Based Colloids and Materials, Department of Bioproducts and Biosystems, Aalto
University, FI-00076 Aalto, Espoo, Finland
4
Biopolymers and Colloids Laboratory, Department of Food Science, University of
Massachusetts, Amherst, Massachusetts 01003, USA
Annu. Rev. Food Sci. Technol. 2021. 12:1.1–1.24 Keywords

The Annual Review of Food Science and Technology is
plant nanocellulose, cellulose nanocrystals, cellulose nanofibrils, Pickering
online at food.annualreviews.org
stabilization, functional foods
https://doi.org/10.1146/annurev-food-061920-
123242 Abstract
Copyright © 2021 by Annual Reviews.
In this article, the application of nanocelluloses, especially cellulose nanofib-
All rights reserved
rils and cellulose nanocrystals, as functional ingredients in foods is re-
viewed. These ingredients offer a sustainable and economic source of nat-
ural plant-based nanoparticles. Nanocelluloses are particularly suitable for
altering the physicochemical, sensory, and nutritional properties of foods
because of their ability to create novel structures. For instance, they can
adsorb to air–water or oil–water interfaces and stabilize foams or emul-
sions, self-assemble in aqueous solutions to form gel networks, and act
as fillers or fat replacers. The functionality of nanocelluloses can be ex-
tended by chemical functionalization of their surfaces or by using them
in combination with other natural food ingredients, such as biosurfactants
or biopolymers. As a result, it is possible to create stimuli-responsive, tai-
lorable, and/or active functional biomaterials suitable for a range of food
·.•�-
1.1
, Review in Advance first posted on

December 9, 2020. (Changes may
still occur before final publication.)
FO12CH01_Bai ARjats.cls November 28, 2020 12:24
applications. In this article, we describe the chemistry, structure, and physicochemical properties
of cellulose as well as their relevance for the application of nanocelluloses as functional ingredients
in foods. Special emphasis is given to their use as particle stabilizers in Pickering emulsions, but we
also discuss their potential application for creating innovative biomaterials with novel functional
attributes, such as edible films and packaging. Finally, some of the challenges associated with us-
ing nanocelluloses in foods are critically evaluated, including their potential safety and consumer
acceptance.
INTRODUCTION
Nanotechnology has been widely promoted for its potential to improve human health and well-
being and has attracted considerable attention in the agriculture and food sectors (Patel 2018).
Food-grade nanomaterials may be naturally present in edible foodstuffs, produced during normal
food-processing operations, or intentionally incorporated into foods as functional ingredients.
The food industry may utilize the unique physicochemical properties of nanoparticles, such
as their small dimensions and large surface areas, to improve food safety, quality, nutrition, or
function (DeLoid et al. 2018). Nevertheless, it is important to consider the potential adverse
effects associated with nanomaterials when utilizing them as food ingredients (Peters et al. 2016).
Nanocelluloses are prime examples of environmentally friendly nanomaterials that are available
from natural, renewable, and sustainable plant-based sources (Habibi et al. 2010). There is
growing interest in identifying new plant-based ingredients in foods to replace animal-based or
synthetic ones because of consumer demands for healthier and more sustainable food products
(McClements et al. 2017). Nanocelluloses are particularly suitable for this purpose because they
can be used to modulate the physicochemical and sensory attributes of foods, especially their
appearance, texture, and stability (Osorno & Castro 2018).
In this article, we briefly discuss the chemistry and structure of nanocelluloses in their natural
environment and foods. We then provide an overview of recent advances in the utilization of
nanocelluloses as functional ingredients in foods, focusing on their application as additives in
food emulsions and as structural components in packaging materials. Finally, we introduce some
of the potential challenges of using nanocelluloses as functional food ingredients, particularly
their safety profile.
NANOCELLULOSES
Chemistry and Structure of Celluloses
Cellulose is a renewable, sustainable, and biodegradable polymer that can be economically isolated
from many plant sources (Klemm et al. 2005). In their natural environment, cellulose molecules are
packed into tough, water-insoluble fibrous materials that are the main load-bearing components
in the cell walls of plants (Habibi et al. 2010). Cellulose is a high-molecular-weight homopolymer
consisting of β-1,4-linked anhydro-d-glucose units, in which every unit is corkscrewed 180° with
respect to its neighbors (French 2017). Each cellulose molecule possesses chemical asymmetry
because there is a reducing group at one end and a nonreducing group at the other end (Hieta
et al. 1984).
In plants, cellulose molecules interact with each other to form multilevel hierarchical struc-
tures consisting of nested bundles of microfibers (Figure 1a) (Y. Li et al. 2018), which are gen-
erated during the plant’s biogenesis process (Somerville 2006). Typically, 36-, 24-, or 18-chain
·.•�-
(elementary) microfibrils assemble into larger units, which then pack into still larger entities, and
1.2 Bai et al.

a
Tree Cellular structure Cell/fiber CNF aggregate CNF Cellulose
m
O
H
0.5 nm
O OH
H H
Secondary wall
CH2OH H
S3
H OH
on
illati O
Fibr H
Ordered HO O
S2 H
H
H CH2OH
HO H
S1 O
Disordered Hyd
Prima roly
r y wall sis
20–4
0 μm
CNC
cm 10 nm
b c d e
~7 nm
20 nm
010
f 1-1
0 OH
110 CH2
200
200 nm 500 nm
Hydrophilic
Hydrophobic
Figure 1
(a) Schematic illustration of the isolation of cellulose nanocrystals (CNCs) and cellulose nanofibrils (CNFs) from wood and other plant
sources. Panel a adapted with permission from Y. Li et al. (2018); copyright 2018 Wiley-VCH. (b) Transmission electron microscopy
(TEM) of rod-like CNCs. (c) TEM of longer CNFs typically forming percolative structures in water. (d) Schematic illustration and
electron tomography image of chiral CNCs with 7-nm diameters. Panel d adapted with permission from Majoinen et al. (2014);
copyright 2014 American Chemical Society. (e) Visual appearance of CNC film upon drying, showing structural color (green). ( f )
Different planes of microfibril structure, exhibiting different levels of hydrophilicity. Panel f (left) adapted with permission from Dri
et al. (2013); copyright 2013 Springer. Panel f (right) adapted with permission from Kalashnikova et al. (2012); copyright 2012
American Chemical Society.
these in turn form the cellulose fibers. The cellulose chains are primarily held together by van
der Waals forces, hydrogen bonds, and hydrophobic interactions (Medronho et al. 2012). How-
ever, the precise mechanisms leading to the formation of a cellulose structure, i.e., its biosynthesis
and assembly, are still being debated (Brown 2004, Rongpipi et al. 2019). It has been proposed
that disordered regions exist in cellulose fibers, which may be distributed as chain dislocations on
segments along the elementary fibrils, where the microfibrils are distorted by internal strain in
the fiber causing them to tilt and twist (Habibi et al. 2010). In the ordered regions, the cellulose
molecules are tightly packed together into crystallite structures via strong hydrogen bonds within
and between the chains (Agarwal et al. 2016).
Classification of Nanocelluloses
Cellulose nanofibrils (CNFs) or cellulose nanocrystals (CNCs) can be isolated from wood and
·.•�-
other plant sources by partial disruption of their natural structures, which is usually achieved using
www.annualreviews.org • Plant-Based Nanocelluloses in Foodstuffs 1.3

chemical and/or mechanical treatments. Besides plants, some bacteria naturally produce cellulose
microfibrils, which are referred to as bacterial nanocelluloses (BNCs) (Montoya et al. 2019). These
three types of nanocelluloses (CNCs, CNFs, and BNCs) have different morphologies (sizes and
shapes) depending on their biological origin and the processes used to isolate them. The current
review focuses on plant-derived nanocelluloses. The properties and food applications of BNCs
are addressed in recent comprehensive reviews (Osorio et al. 2017, Ullah et al. 2016).
CNCs are typically produced from cellulose fibers after selective removal of the less-ordered
domains present in the source material, for example using controlled acid hydrolysis, which leaves
the crystalline domains intact (Habibi et al. 2010). The resultant nanoparticles are rigid nanorods
showing high crystallinity (Figure 1b) (Klemm et al. 2011). In aqueous suspensions, CNCs self-
assemble into nematic liquid crystals above a critical concentration because of their inherent chi-
rality (Figure 1d) (Revol et al. 1992). Upon drying, these hierarchical structures are retained, lead-
ing to the formation of tightly packed solid films that exhibit selective light reflection or structural
color (Figure 1e) (Klockars et al. 2018). It should be noted that CNCs are sometimes also referred
to as nanocrystalline celluloses (NCCs) or cellulose nanowhiskers (CNWs).
The most widely used means of producing CNCs involves sulfuric acid hydrolysis (Rånby
1951). This method leads to the generation of sulfate half-ester groups on the surfaces of the cel-
lulose molecules, which enhances the colloidal stability of CNCs in aqueous media due to strong
electrostatic repulsion between the negatively charged particles. Other acids or oxidizing agents
have also been used to produce CNCs with surface carboxyl groups (Chen et al. 2016) or phos-
phate half-esters (Camarero Espinosa et al. 2013). Hydrolysis of cellulose using hydrochloric acid
leads to the creation of uncharged CNCs, which are unstable to aggregation in water because of a
lack of electrostatic repulsion (Araki et al. 2001). Researchers have shown that hydrochloric acid
vapor can be used to simplify the laborious purification and acid recycling steps involved in CNC
manufacture, while still achieving a high yield and low production costs (Kontturi et al. 2016).
CNFs are usually obtained by disintegrating the cell walls of the fibers using high-energy
mechanical shear, which leads to particles that are longer and less crystalline than the CNCs
(Figure 1c) (Kontturi et al. 2018). The morphology and surface chemistry of the fibrils formed
depend on the biological origin of the cellulose as well as the process, e.g., carboxymethylation
(Wågberg et al. 2008) or enzymatic treatment (Pääkkö et al. 2007), used to assist the deconstruction
of the cell walls. Catalyzed oxidation of cellulose fibers with 2,2,6,6-tetramethylpiperidine-1-oxyl
(TEMPO) is one of the most efficient methods to isolate small uniform individual nanofibrils,
which are usually referred to as TEMPO-oxidized CNFs (TOCNFs) (Saito et al. 2007). Con-
versely, intensive mechanical shearing, without proper pretreatment, usually leads to a more het-
erogeneous distribution of lateral fibril dimensions, typically a mixture of cellulose microfibrils
and nanofibrils (Bai et al. 2019a). The high axial aspect ratio of these cellulose nanomaterials
promotes intramolecular and intermolecular entanglements, which, together with hydration and
electrostatic interactions (Ling et al. 2018), enables the formation of hydrogels at low concentra-
tions. In addition, these hydrogels often exhibit strong shear-thinning behavior (Nechyporchuk
et al. 2016), which is useful for many applications. It should be noted that CNFs are also sometimes
referred to as nanofibrillated celluloses (NFCs) or microfibrillated celluloses (MFCs).
Nanocellulose Characteristics Relevant to Food Applications

The nanoparticles isolated from cellulose (CNCs and CNFs) naturally have an amphiphilic char-
acter because crystalline cellulose has both hydrophilic and hydrophobic faces (Figure 1f ) (Dri
et al. 2013, Medronho et al. 2012). The amphiphilicity of nanocelluloses means they can be used
·.•�-
to stabilize emulsions and foams by adsorbing to oil–water or air–water interfaces (Kalashnikova
1.4 Bai et al.

et al. 2012). The colloidal nature of nanocelluloses means they can be used to create fat mimetics
by modifying the optical or rheological properties of aqueous solutions. The ability of nanocellu-
loses to self-associate and form particle networks in aqueous solutions means they can be used to
modify the textural attributes of some foods. Finally, the ability of nanocelluloses to create elastic
materials with good barrier properties can be used to create packaging and coating materials with
novel functional properties. It is clear that nanocelluloses are highly versatile ingredients with
many potential applications in foods.
NANOCELLULOSES IN FOOD APPLICATIONS

In this section, some of the most promising potential applications of nanocelluloses within foods
are discussed.
Nanocelluloses as Stabilizers in Food Emulsions

Owing to the inherent nature and promising properties of nanocelluloses, one of their most impor-
tant applications is as stabilizers in food emulsions, which has mainly focused on the oil-in-water
type.
Pickering stabilization. Pioneering work by Ramsden (1904) and Pickering (1907) more than
100 years ago demonstrated that colloidal particles can be used to form and stabilize emulsions.
Emulsions stabilized by colloidal particles are now referred to as Pickering emulsions, despite the
fact that Ramsden published his research work first. The type of emulsion that can be stabilized by
a certain type of colloidal particle depends on its wettability (Binks 2002). For instance, colloidal
particles that are preferentially wetted by water or oil are more suitable for forming oil-in-water
or water-in-oil emulsions, respectively. The interfacial adsorption of particles depends on the syn-
ergy between particle surface chemistry and interfacial tension between the phases, which can be
calculated by the following equation (Binks 2002, Levine et al. 1989):
E = π r 2 γ (1 − |cos θ|)2 .
Here, r is the radius of the colloidal particle (nm), γ is the interfacial tension between the oil and
water phases (N/m), and θ is the contact angle of the particles adsorbed at the oil–water interface.
This equation predicts that the detachment energy of particles from the interface is much higher
than the thermal energy (kB T ) under conditions in which the particles have an approximately
equal affinity for both the oil and water phases (Berton-Carabin & Schroën 2015). As a result,
the colloidal particles can be assumed to be irreversibly adsorbed to the interface, which means
that the oil droplets in Pickering emulsions are highly stable to coalescence (Figure 2a). Once
the colloidal particles are adsorbed at the interfaces, a mechanically robust barrier is formed that
sterically restricts the droplets from approaching each other (Bai et al. 2019c). Indeed, oil droplets
coated by colloidal particles are often much more resistant to coalescence than those stabilized
by molecular emulsifiers. It should be noted, however, that a high level of energy input is often
required to form Pickering emulsions so as to overcome an adsorption energy barrier that opposes
the initial particle absorption. Many studies have shown that synthetic spherical and rod-like par-
ticles can be used to stabilize emulsion droplets by this mechanism (Figure 2b,c) (Dinsmore et al.
2002, Zhou et al. 2009). But recently there has been great interest in the use of natural colloidal
particles for this purpose. As mentioned earlier, there is a growing demand for label-friendly food
products fabricated from natural plant-based ingredients (Bai et al. 2016, McClements et al. 2017).
·.•�-
Nanocellulose shows particular promise in forming and stabilizing food emulsions because of its

a b c
Water
phase
Oil High-energy input
phase upon particle adsorption
ΔE >> k BT
θ
2 μm 20 μm
Figure 2
(a) Schematic illustration of the adsorption of particles at the water–oil interface with a contact angle smaller than 90° (oil-in-water
emulsion). The adsorption of particles to the interfaces requires additional energy input upon Pickering stabilization. (b) Scanning
electron microscopy (SEM) of spherical polystyrene particles adsorbed at the oil–water interfaces. Panel b adapted with permission
from Dinsmore et al. (2002); copyright 2002 American Association for Advancement of Science. (c) SEM for rigid rod-like particles
assembled on a bubble. Panel c adapted with permission from Zhou et al. (2009); copyright 2009 Wiley-VCH.
strong surface activity, good film-forming properties, sustainability, biodegradability, and nontox-
icity (Bai et al. 2019a).
Nanocelluloses as emulsion stabilizers. The emulsion-stabilizing properties of nanocelluloses

depend on many factors, including their thickness, length, surface chemistry, and surface charge
(Bai et al. 2019a). Nanocelluloses are typically more hydrophilic than hydrophobic, which means
that they are usually used to stabilize oil-in-water emulsions (Berton-Carabin & Schroën 2015).
However, water-in-oil emulsions can be generated using modified nanocelluloses (Guo et al. 2017).
Rod-like CNCs isolated from cotton, bacteria, algae, and other bioresources have been shown to
irreversibly adsorb at the oil–water interface to form stable emulsions (Kalashnikova et al. 2013,
Kasiri & Fathi 2018). The aspect ratio (length-to-width ratio) of CNCs has been shown to influ-
ence the surface coverage of oil droplets, with denser packing for short rods and looser packing for
long rods (Kalashnikova et al. 2013). Long, flexible CNCs may also promote emulsion stability by
forming a gel network of entangled fibers in the aqueous phase that inhibits droplet movement.
The impact of the surface sulfur content of CNCs on their ability to form and stabilize oil-in-
water Pickering emulsions has been examined (H. Zhang et al. 2019). It was shown that CNCs with
higher surface sulfur content were better at forming and stabilizing the emulsions. The stability of
Pickering emulsions containing flavor oil (d-limonene) droplets coated with corn nanocellulose
has been shown to be highly sensitive to electrostatic effects (Wen et al. 2014). The emulsions
become unstable to creaming at low pH and high-salt concentrations, which has been attributed
to electrostatic screening effects. Conversely, the addition of NaCl prior to homogenization facili-
tated the creation of CNC-stabilized Pickering emulsions with tunable droplet size (Kalashnikova
et al. 2011). This effect was ascribed to the ability of the salt ions to partially screen the negative
charge on the CNCs, thereby promoting adsorption and closer interfacial packing. In other stud-
ies, high-internal-phase Pickering emulsions have been produced using CNCs as emulsifiers in the
presence of low levels of salt (Capron & Cathala 2013). These results demonstrate the importance
of the electrical properties of CNCs for the formation and stabilization of Pickering emulsions.
One of the limitations of using unmodified CNCs to stabilize food emulsions is the relatively
large size of the oil droplets produced, with the smallest droplets being in the micron-range (Bai
et al. 2018a). As a result, these emulsions are highly unstable to gravitational separation (creaming)
during storage (Bai et al. 2017). In a recent study, edible oil-in-water Pickering emulsions were
·.•�-
successfully prepared by high-energy microfluidization using unmodified CNCs as Pickering
1.6 Bai et al.

stabilizers (Bai et al. 2019c). Under optimized homogenization conditions, the mean droplet
diameter produced was less than 1 μm. As a consequence, the creaming stability of the emulsions
was increased substantially, which may be important for many food applications.
Food-grade hydrophobized CNCs have also been proven to be effective at improving emul-
sion stability. For example, food-grade octenyl succinic anhydride (OSA) was recently used to
modify CNCs to improve their emulsifying properties (Du Le et al. 2020b). The oil droplets
in Pickering emulsions formed using OSA–CNC were highly resistant to coalescence, but they
were prone to flocculation when the electrostatic repulsion between them was reduced by alter-
ing the pH or ionic strength. In a recent study, a food-grade, cationic, small-molecular surfactant,
ethyl lauroyl arginate (LAE), was used to modulate the behavior of CNCs at oil–water interfaces,
which enhanced their emulsifying properties (Bai et al. 2018b). The adsorption of CNCs at the
interfaces was influenced by LAE concentration, which was attributed to the formation of in-
terfacial CNC–LAE complexes with different charges, thicknesses, and structural organizations
(Figure 3a), thereby leading to different emulsion stabilization properties (Figure 3b). Under
optimized conditions, the emulsions were highly stable to creaming and coalescence even after
long-term storage, demonstrating the efficiency of using CNCs in combination with an edible
molecular surfactant.
CNFs, which consist of longer filaments than CNCs, have also been used in forming and sta-
bilizing food emulsions. Essential oil emulsions stabilized with carboxylated CNCs and CNFs
were shown to exhibit antibacterial activity against several foodborne pathogens (Mikulcová et al.
2018). The size of the oil droplets formed was larger for the emulsions stabilized with CNFs than
the ones stabilized with CNCs. In contrast, the CNF emulsions were more stable to creaming
than the CNC emulsions, which was attributed to the formation of a gel network by the long
CNFs. This phenomenon has also been observed in other studies on the rheological properties of
CNF-stabilized Pickering emulsions (Winuprasith & Suphantharika 2015). Recent studies have
examined the impact of CNF type on the formation of stable Pickering food emulsions, which
found that different CNF ingredients had different functionalities (Li et al. 2019a,b).
Enhancement of nanocellulose performance using ingredient interactions. The functional

performance of nanocelluloses can be extended by using different combinations of them, or by us-
ing them in combination with other natural ingredients. For example, highly stable food emulsions
have been created using a mixture of CNCs and CNFs (Bai et al. 2018a). The CNCs preferentially
adsorbed to the surfaces of the oil droplets and stabilized them against coalescence, whereas the
CNFs promoted the formation of a 3D network of aggregated oil droplets and polymers in the
emulsions that provided mechanical strength and inhibited gravitational separation. At an opti-
mum CNF concentration, the emulsions were stable for more than 6 months without showing any
sign of separation, satisfying the shelf-life requirements for many food products, such as dressings
or sauces. In another study, Pickering emulsions that were stable to dehydration and rehydra-
tion were produced using a combination of CNCs, tannic acid (TA), and water-soluble cellulose
derivatives (Hu et al. 2016). Initially, Pickering emulsions that were stable to creaming and coa-
lescence were produced by mixing CNCs with either methyl cellulose or hydroxyethyl cellulose.
Subsequently, TA was incorporated into the emulsions to improve their stability to freeze-drying
and rehydration. The underlying mechanism involved the formation of complexes between the
cellulose derivatives and TA at the oil droplet surfaces, leading to the formation of a protective
shell around them. As a consequence, the oil droplets were readily rehydrated without the need
for high-energy mixing and without a large change in droplet size before or after rehydration.
This type of emulsion can be produced using all-natural ingredients, which may be an advantage
·.•�-
for some food applications.

1,800
a I II III IV
LAE
1,600
1,400
No CNCs
ΔH (μcal/injection)
1,200
CNC I Electrostatic attraction II Surface reorganization
1,000
CNCs
800
600
400
200
0
0.00 0.05 0.10 0.15 0.20 0.25 0.30

IV Free LAE micelles III CNC-induced micellization
Lauric arginate concentration (wt%)
20 μm 20 μm 20 μm
CNC/LAE
complex
to and
Low LAE Medium LAE High LAE
Figure 3
(a) Enthalpy change integrated from heat flow in isothermal titration calorimetry (left) and schematic illustration showing complex
formation (right) as a function of ethyl lauroyl arginate (LAE) concentration in a cellulose nanocrystal (CNC) suspension. (b) Confocal
images (upper) and illustration (lower) of Pickering droplets stabilized by CNC–LAE complexes at varied LAE loading levels. Figure
adapted with permission from Bai et al. (2018b); copyright 2018 Royal Society of Chemistry.
Recently, mixed Pickering emulsions have been prepared by blending two types of oil droplets
coated by different nanoparticles, one stabilized by anionic CNFs and the other by cationic
nanochitin (NCh) (Zhou et al. 2019). Emulsions with tunable properties can be produced by vary-
ing the ratio of anionic and cationic oil droplets. The net charge and size of the composite particles
formed in these emulsions depend on the mixing ratio, thereby influencing their functional perfor-
mance (Bai et al. 2019b). Under appropriate conditions, composite particles can be formed that
consist of a shell of NCh-coated droplets around CNF-coated droplets. Mixed emulsions were
found to have better coalescence stability than single emulsions containing only CNF-coated
·.•�-
droplets. This approach may be useful in the production of highly stable food emulsions with
1.8 Bai et al.

tailorable textural and sensory properties. Other recent studies have shown that the emulsifying
properties of CNFs can be improved by using them in combination with soy protein (X. Zhang
et al. 2019), guar gum, or carboxymethyl cellulose (Golchoobi et al. 2016). There is therefore
considerable scope for creating food emulsions with novel functional attributes based on careful
control of interactions between CNFs and other natural food components.
Ingredient interactions can also be used to extend the performance of nanocelluloses in other
types of colloidal systems. Water-in-water (W/W) Pickering emulsions have been stabilized by us-
ing CNCs to adsorb to the interface between two phase-separated aqueous phases formed by mix-
ing dextran and poly(ethylene oxide) in water (Peddireddy et al. 2016). This W/W emulsion con-
sisted of a poly(ethylene oxide)-rich dispersed phase and a dextran-rich continuous phase, with the
CNCs being mainly present at the interfaces and in the continuous phase. The addition of NaCl
to these emulsions led to the formation of weak gels in the continuous phase because of cross-
linking of the nonadsorbed CNCs, which arrested the creaming of the dispersed phase droplets,
thereby improving emulsion stability. In another study, CNC-stabilized water-in-water emulsions

were prepared with controllable gelation rate and stiffness (Ben Ayed et al. 2018). The aggrega-
tion rate of CNCs in the continuous phase could be controlled by adding different amounts of
NaCl. At sufficiently high aggregation rates, emulsion gels were formed that were highly resistant
to creaming, which was ascribed to the formation of a 3D network of CNCs.
Functional Properties of Nanocellulose in Foods

In this section, we review some of the most promising applications of nanocellulose as a functional
ingredient in foods.
Modulation of gastrointestinal fate. Emulsion technology is particularly suitable for the de-
velopment of functional foods and beverages designed to improve human health and well-being
(McClements 2020). In this section, the potential of nanocelluloses to enhance the health bene-
fits of food emulsions is highlighted. They are particularly suitable for this purpose because they
are nondigestible surface-active materials that can interact with various components within the
human gastrointestinal tract (GIT) (Sarkar et al. 2018). Consequently, they can form physical bar-
riers that prevent digestive enzymes from reaching macronutrients, or they can reduce the activity
of digestive enzymes, bile acids, or other gastrointestinal components by binding to them.
The gastrointestinal fate of CNC-stabilized corn oil–in–water Pickering emulsions was stud-
ied recently using an in vitro GIT model that simulates the mouth, stomach, and small intes-
tine phases (Bai et al. 2019d). The final amount of free fatty acids released from the emulsions
was approximately 40% less when the lipid droplets were coated by CNCs than by gum arabic
(Figure 4a). Presumably, the nanocellulose coating formed around the lipid droplets inhibited
their digestion by blocking the adsorption of bile salts and lipase to the oil–water interface. In an-
other study, the uptake of digested CNC-stabilized oil-in-water Pickering emulsions by murine in-
testinal mucosa was evaluated (Mackie et al. 2019). These results showed that CNCs were trapped
in the intestinal mucus layer and failed to reach the underlying epithelium, i.e., they were not ab-
sorbed. In summary, these results suggest that CNCs can be used to modulate the digestion of
Pickering-emulsified lipids, which may be useful for the development of functional foods.
Other researchers have also examined the ability of nanocelluloses to alter digestion processes.
Extending the function of nanocelluloses in digestion control, researchers at Harvard used a
combination of in vitro (simulated GIT and cell culture) and in vivo (animal feeding) models to
investigate the impact of nanocellulose on lipid digestion and absorption (DeLoid et al. 2018).
·.•�-
They reported a 36% reduction in blood triglyceride levels in the animals when the lipids were

100
100
a 95 b Bioaccessibility (%)
Free fatty acids released (%)
Stability (%)
90
50
Vitamin D3 level (%)

85
80
40
75
30 70
Gum arabic 65
0.1 wt% CNC 0.5 wt% CNC
20 60
0.2 wt% CNC 0.75 wt% CNC
0.3 wt% CNC 1.0 wt% CNC 55
0 50
0 20 40 60 80 100 120 0.1% CNF 0.3% CNF 0.5% CNF 0.7% CNF 0.7% WPI
Time (min)
Figure 4
(a) Free fatty acids released as a function of time during simulated small intestinal digestion of cellulose nanocrystal (CNC)-stabilized
corn oil–in–water Pickering emulsions. The emulsions were stabilized at different loading levels of CNCs, and the results compared to
those after stabilization with 0.75-wt% gum arabic. Panel a adapted with permission from Bai et al. (2019d); copyright 2019 Elsevier.
(b) Influence of emulsifier type and concentration on vitamin D3 stability and bioaccessibility in oil-in-water emulsions stabilized by
either cellulose nanofibrils (CNFs) or whey protein isolate (WPI) in a simulated digestion model. Panel b adapted with permission from
Winuprasith et al. (2018); copyright 2018 Elsevier.
co-ingested with 1% nanocellulose. This effect was attributed to two primary mechanisms:
(a) the coalescence of fat droplets on fibrillar nanocelluloses (Figure 5a), resulting in a reduction
of the available surface area for lipase binding, and (b) sequestration of bile salts, causing impaired
interfacial displacement of proteins at the lipid droplet surface and impaired solubilization of
lipid digestion products (Figure 5b). Another recent study investigated the influence of adding
nanocelluloses (CNCs, CNFs, and TOCNFs) to preexisting emulsions on the lipid digestion of
emulsions under simulated GIT conditions (Liu et al. 2019). All three nanocelluloses inhibited
lipid digestion by an amount that depended on the type and level added.
Pickering emulsions stabilized by hydrophobically modified CNCs have also been used as de-
livery systems for short-chain fatty acids, which may have beneficial effects on colon health (Du
Le et al. 2020a). The presence of CNC coating inhibited the digestion of the lipid droplets under
simulated gastrointestinal conditions, which should lead to a higher concentration of short-chain
fatty acids reaching the colon. The impact of nanocelluloses on the bioavailability of micronutri-
ents encapsulated within emulsions has also been examined. The effect of CNFs on lipid digestion
and vitamin D3 bioaccessibility in Pickering emulsions has recently been investigated using a sim-
ulated GIT model (Winuprasith et al. 2018). The rate and extent of lipid digestion decreased as
the CNF concentration increased, which was attributed to the ability of the nanocellulose to in-
hibit the interactions of the lipase with the lipids. The bioaccessibility of vitamin D3 also decreased
with increasing CNCs because the lipid phase was not fully digested and thus some of the vita-
mins were not released and there were fewer mixed micelles to solubilize them (Figure 4b). These
results show promise in food-based treatments by, e.g., using nanocellulose-stabilized Pickering
emulsions in targeted delivery, which, e.g., passes the harsh environments in the stomach, small
intestine, and colon.
Modulation of structural and textural properties. Nanocelluloses can also be used as natural
additives in foods to alter the structure and texture of food products. Nanocelluloses have been
·.•�-
used to stabilize sauces and milkshakes by increasing their viscosities (Okiyama et al. 1993). They
1.10 Bai et al.

Pure cream Cream/CNF

a
Before digestion
Fat
Fat
2 μm 2 μm
CNF
After digestion
CNF
Fat
Fat
2 μm 2 μm
b Without nanocellulose With nanocellulose
Nanocellulose
Fat
Lipase
Protein
Bile salt
Figure 5
(a) Scanning electron microscopy images of digested products of cream only (left column) and cream with
cellulose nanofibrils (CNFs) (right column). The upper row shows images at the start of the small intestinal
phase, and the lower row displays images at the end of the small intestinal phase. (b) Schematic illustration
showing the modulation mechanism of fat digestion in the presence of nanocelluloses. Figure adapted with
permission from DeLoid et al. (2018); copyright 2018 American Chemical Society.
have also been used to modulate the gelation characteristics of chicken breast in the absence and
presence of a protein cross-linking agent [transglutaminase (TG)] (Zhang et al. 2018). The pres-
ence of nanocellulose increased the water-holding capacity of the gels, which can be attributed to
·.•�-
its ability to form a 3D-hydrogel network that holds in water through capillary forces.

a Na CNF b 680 665.2
Calorie (kJ/100 g)
Micelle
COO – 640 627.6
600 589.9
552.3
560
0 10 20 30
Replacement of cream (%)
51.38
Melting rate (%)

50
40 500 μm
32.21
30 27.79
21.98
20
0 10 20 30
Replacement of cream (%)
Figure 6
(a) Schematic illustration (not to scale) of bridged cellulose nanofibrils (CNFs) by surfactant micelles. Constituent sizes (diameters, d)
are dNA+ ≈ 0.4 nm, dmicelle ≈ 10 nm, and dCNF ≈ 10 nm. The length of CNFs is approximately equal to 1 μm. Free micelles are
represented in green and the micelles establishing CNF junctions are depicted with a red corona as seen in the inset. Panel a adapted
with permission from Quennouz et al. (2016); copyright 2016 Royal Society of Chemistry. (b) Calculated calories (upper panel) and
melting rate (bottom panel) of ice creams at varied levels of CNF/soy protein isolate replacements. Panel b adapted with permission from
Sun et al. (2015); copyright 2015 Springer.
Nanocelluloses have also shown the capability to alter the rheological properties of model fluid
foods (Nechyporchuk et al. 2016). CNFs have a high aspect ratio, which means that they can form
percolated gel networks at very-low-mass concentrations (Aaen et al. 2019). The texture modifying
properties of these dilute CNF suspensions can be modulated by adding surfactants that interact
with them (Figure 6a) (Quennouz et al. 2016). At low surfactant levels, the gel strength increases
and the gel remains optically clear, but at high surfactant levels there was a loss of suspension
stability and a reduction in optical clarity. This transition was driven by increasing bridging of the
nanofibrils by the surfactant micelles.
Recently, CNFs have been used to modify the structure and performance of standard and low-
fat ice cream formulations (Velásquez-Cock et al. 2019). The viscosity of both standard and low-fat
ice cream premixes was increased after CNF addition, whereas the behavior of the frozen products
differed according to the fat content. Standard formulations showed higher fat destabilization,
longer melting onset times, and reduced melting rates. Low-fat formulations showed no significant
changes in fat destabilization and melting onset times. These results suggest that the impact of
CNFs depends on their ability to interact with the fat droplets and structure the aqueous phase.
The sensory attributes of the low-fat samples were improved after the addition of CNFs, even
after heat shocking the sample. Interestingly, the hardness of the frozen ice cream (<−2°C) was
not affected by CNF addition, which was attributed to the fact that it did not impact ice crystal
growth.
One of the main goals of modern food technology is to create healthier processed foods, such as
foods with lower energy densities designed to tackle obesity and other diet-related chronic diseases
(McClements 2020). Nanocellulose is a promising ingredient for the formulation of these kinds
·.•�-
of food (Peng & Yao 2017). Amorphous cellulose, which is capable of retaining a high amount of
1.12 Bai et al.

water, has been used to reduce the fat content and energy density of cheese, hamburgers, baked
goods, and sausages (Robson 2012). Microcrystalline cellulose has been used as a fat substitute in
hamburgers and sausages, reducing their calorie content without adversely impacting their quality
attributes (Gibis et al. 2015). Nanocelluloses have also been used to reduce the energy density of
chocolate (Watson et al. 2013) and baked goods (Serpa et al. 2016), without impacting their sensory
attributes. A combination of CNFs and soy protein has been used to form gel-like substances that
can replace some of the fat in creams (Sun et al. 2015). Indeed, at optimized CNF concentrations,
the textural characteristics of the reduced-fat creams were very similar to those of conventional
creams. These reduced-fat creams could be used to formulate low-calorie ice creams with desirable
textural properties (Figure 6b).
Apart from the use of nanocelluloses as nondigested dietary fiber, they have been considered
for enabling antimicrobial activities (Tavakolian et al. 2020). Biocompatible and renewable an-
timicrobial agents can be incorporated in hydrophilic nanocellulose carriers for potential food
applications, namely, to assist in the encapsulation and, afterward, in the release of the agents ( J.
Li et al. 2018). Recently, a microencapsulation carrier for sweet orange essential oil was synthe-
sized by combining gum arabic, maltodextrin, and CNFs (de Souza et al. 2018). CNFs acted as
a thickener to increase emulsion viscosity and reduce droplet size. CNFs showed the best en-
capsulation efficiency and released more essential oil at ambient temperatures. This confirms the
function of nanocelluloses as promising excipients with potential antimicrobial ability in foods.
Nanocellulose as Food Packaging Materials

Food packaging is used to protect foods from their environment, thereby extending their shelf
life, improving their quality, and enhancing their safety. To achieve these goals, food packaging
materials must meet certain specifications in terms of their optical, mechanical, barrier, and an-
timicrobial properties (Khan et al. 2014). The barrier properties are crucial for controlling the
exchange of gases and liquids (such as oxygen and water) between the packaged food and its envi-
ronment, thereby reducing chemical, physical, or microbiological degradation. In particular, the
oxygen and water-vapor permeabilities of packaging materials strongly impact the oxidative and
microbial stability of foods. The materials should also have limited water solubility so as to avoid
disintegration when they come into contact with wet surfaces or humid atmospheres. The op-
tical properties of packaging materials, such as their clarity and color, is also important because
it impacts the visual appearance of the product. Ideally, packaging materials should be abundant,
economic, scalable, sustainable, environmentally friendly, and nontoxic.
Currently, most materials used for food packaging are produced from nonrenewable and non-
biodegradable resources, which leads to serious environmental problems. A considerable research
effort has been made to develop biodegradable packaging materials from renewable resources
(Mohamed et al. 2020). However, the biomaterials produced often do not exhibit the desir-
able functional performance that can be achieved with synthetic materials. Nanocelluloses show
great promise for improving the functional attributes of more ecofriendly packaging materials
(Ferrer et al. 2017) as well as creating novel functional attributes in advanced packaging materials
(Vilarinho et al. 2018).
Improvement of packaging properties using nanocellulose. In this section, the utilization of

nanocellulose to improve the performance of food packaging materials is discussed (Li et al. 2015).
CNFs have been used to improve the mechanical and barrier properties of mango puree–based
edible films (Azeredo et al. 2009). Edible packaging films were prepared by loading nanocellu-
loses at different concentrations into mango puree and then drying the obtained mixture. The
·.•�-
presence of CNFs increased the tensile strength and Young’s modulus of the films, which was

mainly attributed to the formation of a network of aggregated CNFs within the matrix. The addi-
tion of CNFs also improved the barrier properties of these films, presumably by increasing their
tortuosity. In a recent study, a facile, green, and sustainable method of fabricating mechanically
robust packaging materials was reported by incorporating zein nanoparticles into CNF networks
(Li et al. 2020). The nanocomposite films formed had good mechanical properties and thermal
stability, i.e., the protein nanoparticles behaved as active fillers, which was attributed to strong
attractive interactions between the zein nanoparticles and the CNF matrix. The antimicrobial ac-
tivity of these films was also enhanced by incorporating nonpolar antimicrobial agents within the
zein nanoparticles.
Nanocelluloses have also been used to enhance the mechanical and barrier properties of
alginate–acerola puree films (Azeredo et al. 2012). The overall tensile properties and water-vapor
barrier of alginate-acerola puree films were improved by an amount that depended on the nature
of the nanocellulose used. Nanocellulose extracted from coconut fiber was more effective than that
extracted from cotton husk, which was ascribed to differences in their aspect ratios. Recently, the
impact of nanocellulose on the properties of cassia gum (CG) films was investigated (Cao et al.
2020). The heat-sealing, barrier, and mechanical properties of the CG-based edible films were
improved by incorporating optimized amounts of nanocellulose within them. These effects were
mainly attributed to hydrogen bonding between the cassia gum and nanocellulose.
The impact of casein (a milk protein) on the mechanical properties of nanocomposites compris-
ing CNFs and polylactic acid (PLA) has been studied (Khakalo et al. 2018). The tensile strength
and Young’s modulus of the nanocomposites were significantly increased in the presence of the
casein, which was attributed to its ability to enhance the dispersion of the CNFs within the PLA
matrix (Khakalo et al. 2017). It should be noted that the mechanical strength of packaging ma-
terials is not their only important rheological property. The ductility, or ability to be stretched
without breaking, of packaging materials must also be carefully controlled for certain applications
(Huan et al. 2018). Therefore, a more comprehensive understanding of the impact of nanocel-
luloses on the overall mechanical properties of food packaging materials should be the focus of
future research.
Packaging films comprising nanocellulose often have excellent oxygen barrier properties
(Azeredo et al. 2017). This effect is attributed to the ability of the nanocellulose to form densely
packed solids held together by strong hydrogen bonding (Svagan et al. 2016). As a result, there
is a major suppression of molecular diffusion through the nanocellulose matrix due to tortuosity
effects, i.e., an increase in the path length (Dhar et al. 2015). For this reason, nanocelluloses are
widely used to modify the oxygen permeability of food packaging materials. Nanocelluloses can
also decrease the water-vapor permeability of nanocomposite films assembled from different re-
newable sources, such as poly(vinyl alcohol) (Paralikar et al. 2008) and chitosan (Khan et al. 2012).
The impact of moisture on the behavior of packaging films can also be tuned using nanocellu-
loses (Kriechbaum & Bergström 2020). Nanocelluloses have been shown to increase the water
resistance of films made from other biopolymers, such as alginate (Abdollahi et al. 2013), starch
(Chen et al. 2009), and soy protein (Wang et al. 2006). This effect is partly due to strong hydrogen
bonding between the nanocellulose and the surrounding biopolymer matrix, which enhances the
cohesiveness of the resulting nanocomposites. More details on the application of nanocelluloses in
improving the functional performance of food packaging materials and edible films can be found
in a recent review (Helanto et al. 2019).
Nanocelluloses for active packaging. There is growing interest in the development of a new
generation of packaging materials with novel functional attributes that go beyond those found
·.•�-
in conventional packaging materials (Mei & Wang 2020). At present, the most widely studied
1.14 Bai et al.

active-packaging systems are designed to release active compounds, such as antimicrobial or

antioxidant agents, throughout food storage, thereby increasing the quality and shelf life of the
product (de Azeredo 2013). Nanocelluloses have been shown to be valuable functional ingredients
for the creation of these active-packaging materials (Khan et al. 2014). Recently, a strong and
sustainable food packaging material was developed using CNFs and tannin (Missio et al. 2018).
The CNFs were used to provide good mechanical and barrier properties to the films, whereas
the tannin was mainly used as a natural antioxidant. However, the tannin was also shown to
increase the density and hydrophobicity of the CNF films, which improved their gas-barrier
properties. The authors showed that the tannin was slowly released from the films when they
were in contact with water. Biodegradable nanocomposite films have also been produced from
nanocelluloses and polypyrrole, which were shown to have good antioxidant activity as well as
good barrier properties against oxygen, carbon dioxide, and water vapor (Bideau et al. 2017). The
observed improvement in antioxidant activity and barrier properties of the films was attributed
to the coating of polypyrrole on the dense CNF network.

Numerous approaches have been developed to increase the antimicrobial activity of
nanocellulose-based packaging materials, including incorporating antimicrobial metal nanopar-
ticles (Wu et al. 2019), essential oils (Sogut 2020), cationic biopolymers (Dehnad et al. 2014), and
phytochemicals (Moreirinha et al. 2020). As an example, the impact of nanocellulose and silver
nanoparticles on the physical properties and antimicrobial activity of poly(vinyl alcohol)-based
films has been investigated (Sarwar et al. 2018). The resulting nanocomposite films had high an-
timicrobial activity, improved physical properties, and low cytotoxicity, which are useful attributes
for food packaging materials. Recently, active-packaging materials with good mechanical and bar-
rier properties have been formulated from chitosan, β-cyclodextrin citrate, and nanocellulose com-
posites (Adel et al. 2019). The antimicrobial and antioxidant activities of these nanocomposites
were then enhanced by adding clove oil, which is a natural essential oil.
Pickering emulsions stabilized by nanocelluloses have also been used as components in the for-
mulation of active-packaging materials (Deng et al. 2018). For example, CNC-coated bergamot
oil droplets have been incorporated into whey protein films (Sogut 2020). The introduction of
the essential oil droplets improved the mechanical properties and water-vapor permeability of the
films as well as improving their antimicrobial and antioxidant activity. CNF-based edible com-
posite films have also been developed by the solvent casting of soybean oil–in–water emulsions
stabilized by CNFs (Valencia et al. 2019). Flexible, transparent, thermally stable, and biodegrad-
able composite films were obtained at an optimized oil concentration. These films had multilay-
ered structures consisting of oil phases trapped between two layers of CNFs, which significantly
increased the mechanical and wetting properties of the films (Figure 7a). These films dissociated
when placed in water, which should make them biodegradable (Figure 7b). The encapsulation of
curcumin within these composite films increased their antioxidant and antimicrobial activity.
Nanocelluloses can also be used to obtain other desirable functional attributes in packaging ma-
terials. For instance, the optical properties of nanocellulose-based films can be enhanced by con-
trolling the self-assembly of chiral CNCs in aqueous suspensions (Klockars et al. 2018, Majoinen
et al. 2014). Nanocelluloses tend to form nematic liquid crystals in aqueous suspensions, whose
structures are retained after the suspensions are dried to create films. These structures selectively
reflect light waves with different frequencies, thereby leading to permanent structural colors that
are highly resistant to fading. The availability of these naturally colored films could reduce the
amount of synthetic pigments and dyes used in food packaging materials. Nanocelluloses can also
be used to create active-packaging materials with integrated sensors that provide valuable real-
time information about the properties of the food, such as its humidity (Eyebe et al. 2019) or the
·.•�-
presence of specific molecules (Fontenot et al. 2016).

Low oil content
CNF-stabilized
Pickering emulsion Water evaporation
High oil content

b Edible film
10 μm
100 μm
Figure 7
(a) Schematic illustration (not to scale) showing the formation of cellulose nanofibril (CNF)–soybean oil
composite films from Pickering droplets at low and high oil content. (b) Demonstration of the
biodegradability of composite films in water. From left to right, the droplet structure is reformed upon
2-min sonication of the film. Figure adapted with permission from Valencia et al. (2019); copyright 2019
American Chemical Society.
CHALLENGES TO APPLYING NANOCELLULOSES IN FOODS

There are several potential challenges to incorporating nanocelluloses into foods, such as their
potential toxicity, regulatory status, and consumer acceptance. In this section, a brief overview of
the major challenges is provided.
Safety Aspects
Conventional forms of cellulose and their derivatives, such as methylcellulose, are recognized as
generally regarded as safe (GRAS) for use as food ingredients in the United States by the Food
and Drug Administration. At present, the FDA does not regulate new ingredients because they
are nanomaterials. Instead, it takes a science-based regulatory approach that focuses on the safety
aspects of any new food ingredient or product that might be expected to behave differently from
conventional forms. The FDA (2018) states that “food additives are considered safe when there
is a reasonable certainty of no harm from their intended use.” In the case of nanocelluloses, there
is evidence that they alter the gastrointestinal fate of foods, such as reducing macronutrient di-
gestibility and micronutrient bioavailability, in a manner that may be different from their conven-
tional counterparts (Ong et al. 2017). Consequently, it is important to establish their safety profile
to ensure their safe use in food applications.
Studies using cell culture and animal models have shown that nanocelluloses exhibit little cy-
totoxicity or genotoxicity (Bhattacharya et al. 2017, Vartiainen et al. 2011). For instance, the cy-
·.•�-
totoxicity of CNCs has been assessed against nine different cell lines (Dong et al. 2012). CNCs
1.16 Bai et al.

were found to exhibit no cytotoxic effects against any of the cell lines over the concentration
range (0–50 μg/mL) and exposure time (48 h) used. Moreover, the cellular uptake of the CNCs
by these cell lines was minimal. In general, the biological impact of nanomaterials depends on
their physicochemical and structural characteristics, such as their composition, size, shape, polar-
ity, and charge (Albanese et al. 2012, Menas et al. 2017). For this reason, in vivo experiments have
been carried out to evaluate the impact of aspect ratio and surface chemistry of nanocelluloses on
their toxicity using an embryonic zebrafish model (Harper et al. 2016). This study showed that
nanocelluloses had minimal toxic effects on the embryonic zebrafish and that their aspect ratio
and surface chemistry had little impact on their toxicity.
In contrast, several recent studies have reported that exposure to nanocelluloses can promote
some cytotoxicity (Yanamala et al. 2014) and inflammatory effects (Catalán et al. 2017). In vitro
studies have reported that the metabolic activity and proliferation of the cells within a cell cul-
ture monolayer were impaired only when very high concentrations of CNFs were used (Čolić
et al. 2015). This effect may be related to the biopersistence of CNFs within the cells, which may
have provoked an immune response. On the basis of the evidence presented so far, it appears that
nanocelluloses are not strongly toxic at the concentrations that are expected to be found in foods,
but further studies are required to affirm this.
In particular, studies of the potential toxicity of nanocelluloses are required under more realistic
conditions, e.g., accounting for food matrix and gastrointestinal effects (McClements et al. 2016).
For this reason, a team of researchers at Harvard University conducted comprehensive toxicolog-
ical studies of ingested nanocelluloses in foods using physiologically relevant in vitro and in vivo
methods (DeLoid et al. 2019). The nanocelluloses were passed through an in vitro GIT model
(mouth, stomach, small intestine), using both fasted and fed conditions. A triculture cell model of
the small intestinal epithelium was then used to assess the effect of the digested products on cell
layer integrity, cytotoxicity, and oxidative stress. The researchers reported that the nanocelluloses
caused minimal changes in all these factors. The potential in vivo toxicity of the nanocelluloses
was evaluated using a rat gavage model in which CNFs dispersed in either water or a model food
(cream) was fed to the rats twice weekly for 5 weeks. No significant differences in hematology,
serum markers, or histology were observed between controls and rats given the CNFs. Subse-
quently, the effects of ingested CNFs on gut microbial populations and intestinal function were
explored using an in vivo animal model (Khare et al. 2020). A rat gavage model (feeding with water
or cream, with or without CNFs, for 5 weeks) was used to assess the effect of ingested CNFs on
the fecal microbiome and metabolome, intestinal epithelial expression of cell junction genes, and
ileal cytokine production. It was shown that CNFs altered microbial diversity, selectively reducing
certain species, but had little effect on the fecal metabolome. Moreover, CNFs altered the expres-
sion of epithelial cell junction genes and increased cytokine production. These perturbations may
be caused by an adaptive immune response associated with the biopersistence of CNFs, but no
associated pathology was shown during the study. These results underscored the importance of
understanding the potential implications of nanocelluloses in foods, beyond directly evaluating
their toxicity.
Regulatory Status
Before nanocelluloses are used as functional ingredients in a particular food application, it is crit-
ical to ensure that they are legally acceptable in the country of intended use. The legal status
of nanomaterials varies widely from country to country and should be carefully evaluated when
formulating novel food products. As an example, the European Union mandates that food manu-
facturers label their products if they contain nanomaterials, which are defined as particles having
·.•�-
at least one dimension smaller than 100 nm (based on a number distribution). Many forms of

nanocellulose would fall into this category and would therefore have to be labeled as such. As
mentioned earlier, the FDA does not specifically regulate food ingredients because they are nano-
materials but rather because they may have undesirable biological effects due to the fact that they
behave differently in the body compared to conventional forms of the ingredients. As a result, they
regulate a new ingredient based on the weight of the scientific evidence supporting its safety. As
discussed in the last section, there is an increasing body of evidence about the potential biological
effects of nanocelluloses.
Consumer Acceptance
Even when nanocelluloses can legally be used as functional ingredients in foods, their application
may be limited because of poor consumer acceptance (McClements 2020). Consumers must bal-
ance the potential functional benefits provided by nanocelluloses with their potential health risks
(Catalán & Norppa 2017). Consequently, there is a need to understand what consumers perceive
as beneficial and how they construe risks (Giles et al. 2015). Consumers often make decisions
based on organizations or media outlets that highlight the potential risks of nanoparticles, with-
out having a nuanced understanding of the science involved. Thus, organic nanoparticles often
get lumped together with inorganic nanoparticles, even though they may have different biologi-
cal effects and different safety concerns. In general, consumers will likely be less concerned about
nanocellulose-based packaging materials than nanocellulose-based food additives, as the former
type is not intended for direct consumption.
CONCLUSION AND OPPORTUNITIES

This article has reviewed some of the most important applications of nanocellulose as functional
components in foods and food packaging materials. Both CNFs and CNCs, which mainly differ
in the length of their fibers (aspect ratio), can be used in a wide range of food applications. These
nanomaterials can be isolated from abundant and sustainable natural resources, which makes them
particularly suitable as environmentally friendly plant-based functional food ingredients. In the
future, it will be important to establish the physicochemical processes underlying the functional
attributes of nanocelluloses in foods, such as their ability to alter the optical, rheological, transport,
and stability properties of foods and packaging materials. This knowledge can then be used to
design functional foods with improved physicochemical and sensory attributes. Moreover, it will
be important to establish the impact of nanocelluloses on the gastrointestinal fate of foods, such
as their impact on macronutrient digestibility, micronutrient bioavailability, colonic microflora,
and overall gut health. Finally, further research is still required to establish the acute and chronic
toxicity of different nanocelluloses using short- and long-term in vivo studies. This information
will be important to establish the potential toxicity of these new ingredients and the levels at which
they can be safely used in foods.
DISCLOSURE STATEMENT
The authors are not aware of any affiliations, memberships, funding, or financial holdings that
might be perceived as affecting the objectivity of this review.
ACKNOWLEDGMENTS
The authors acknowledge support from the Canada Excellence Research Chair initiative, the
Canada Foundation for Innovation (CFI), and the European Research Council (ERC) under
·.•�-
the European Union’s Horizon 2020 research and innovation program (ERC Advanced Grant
1.18 Bai et al.

Agreement 788489, BioElCell). This material was also partly based on work supported by the
National Institute of Food and Agriculture, US Department of Agriculture (USDA), Mas-
sachusetts Agricultural Experiment Station (project number 831), and USDA Agriculture and
Food Research Initiative grants (2016-08782).
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cls November 28, 2020 12:24

Annual Review of Food Science and Technology

Long Bai,1,2 Siqi Huan,1,2 Ya Zhu,3 Guang Chu,3

Annu. Rev. Food Sci. Technol. 2021. 12:1.1–1.24 Keywords

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www.annualreviews.org • Plant-Based Nanocelluloses in Foodstuffs 1.3

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Nanocellulose Characteristics Relevant to Food Applications

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NANOCELLULOSES IN FOOD APPLICATIONS

Nanocelluloses as Stabilizers in Food Emulsions

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Nanocelluloses as emulsion stabilizers. The emulsion-stabilizing properties of nanocelluloses

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Enhancement of nanocellulose performance using ingredient interactions. The functional

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0.00 0.05 0.10 0.15 0.20 0.25 0.30

Low LAE Medium LAE High LAE

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thereby improving emulsion stability. In another study, CNC-stabilized water-in-water emulsions

Functional Properties of Nanocellulose in Foods

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Vitamin D3 level (%)

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Pure cream Cream/CNF

b Without nanocellulose With nanocellulose

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a Na CNF b 680 665.2

Melting rate (%)

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Nanocellulose as Food Packaging Materials

Improvement of packaging properties using nanocellulose. In this section, the utilization of

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active-packaging systems are designed to release active compounds, such as antimicrobial or

to the coating of polypyrrole on the dense CNF network.

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Low oil content

High oil content

CHALLENGES TO APPLYING NANOCELLULOSES IN FOODS

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CONCLUSION AND OPPORTUNITIES

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Raman spectroscopy. Cellulose 23:125–44

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