Food Hydrocolloids 57 (2016) 178e186

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Food Hydrocolloids
journal homepage: www.elsevier.com/locate/foodhyd

Review

Vegetable nanocellulose in food science: A review

mez H. c, A. Serpa c, J. Vela
C. Go
squez-Cock a, P. Gan
~a
n a, C. Castro b, L. Ve

lez c,
c, *
R. Zuluaga
a
Facultad de Ingeniería Química, Universidad Pontificia Bolivariana, Circular 1
N
70-01, Medellín, Colombia
b
Facultad de Ingeniería Textil, Universidad Pontificia Bolivariana, Circular 1
N
70-01, Medellín, Colombia
c
Facultad de Ingeniería Agroindustrial, Universidad Pontificia Bolivariana, Circular 1
N
70-01, Medellín, Colombia

a r t i c l e i n f o a b s t r a c t

Article history: The use of nanocellulose as a food additive in 1983 was one of the first applications of this plant-derived
Received 6 November 2015 biopolymer. However, at that time, the product was not commercialized owing to the high energetic cost
Received in revised form of the isolation methods used. Currently, improvements in nanocellulose production allow its
8 January 2016
commercialization. The high surface area and aspect ratio, rheological behavior, water absorption and
Accepted 27 January 2016
absence of cytotoxic and genotoxic properties of nanocellulose facilitate its use in food applications. In
Available online 29 January 2016
this review, three different applications were identified: (i) nanocellulose as a stabilizing agent, (ii)
nanocellulose as a functional food ingredient and (iii) nanocellulose in food packaging. The last is the
Keywords:
Vegetable nanocellulose
most common application of nanocellulose in the food industry. Aiming to demonstrate the potential of
Food additive nanocellulose as a stabilizing and functional food ingredient, relevant publications on uses of nano-
Nanotechnology regulation cellulose in food are examined, focusing on applications of nanocellulose as a food additive and safety
and regulatory issues. Nanocellulose has potential use as a stabilizing agent in food emulsions, as dietary
fiber and to reduce the caloric value of food. Nevertheless, validated standards to characterize the pro-
duced nanostructure, quantify its properties and evaluate its toxicity are still required to answer safety
and regulatory issues to achieve the incorporation of nanocellulose as a commercial product in the food
industry.
© 2016 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 178
2. Vegetable nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
3. Vegetable nanocellulose in food applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
3.1. Nanocellulose as a food stabilizer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 182
3.2. Nanocellulose as a functional food ingredient . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 183
3.3. Nanocellulose in food packaging . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 184
4. Safety and regulatory issues of nanocellulose in food . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 184
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 185
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 185
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 185

1. Introduction

Nanomaterial engineering technologies have the potential to

revolutionize industrial food systems, addressing issues related to
health concerns and sustainability (Szakal et al., 2014). According to
* Corresponding author.
E-mail address: robin.zuluaga@upb.edu.co (R. Zuluaga). the scientific report “Inventory in nanotechnology applications in the

http://dx.doi.org/10.1016/j.foodhyd.2016.01.023
0268-005X/© 2016 Elsevier Ltd. All rights reserved.

mez H. et al. / Food Hydrocolloids 57 (2016) 178e186
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agricultural, feed and food sector”, published by EFSA in 2014, silver,
titanium dioxide and nanoencapsulates represent most of the
nanoparticles used in the food industry in recent years (RIKILT and
JRC, 2014). They are commonly used as food contact material (for
instance, food packaging) and nanoencapsulated or nanosized food
additives. According to the Food and Drug Administration FDA the
term “food additive” refers to any substance that is reasonably
expected to become a component of food (Food and Drug
Administration, 2014). However, a comparison between current
and future applications indicates a trend towards organic nano-
materials, such as vegetable and bacterial nanocellulose (RIKILT and
JRC, 2014).
Vegetable nanocellulose is a nanomaterial extracted from wood,
cotton, natural fibers and lignocellulosic materials. It was first
developed by researchers at the ITT Rayonier Eastern Research
Division Lab in Whippany, USA in 1977, but their work was not
published until 1983 (Turbak, Snyder, & Sandberg, 1983a). Nano-
cellulose has received considerable attention in the following years,
evidenced by the significant rise in the number of scientific articles
and patents published. Most of the scientific articles and patents
developed in recent years about nanocellulose are focused on ap-
plications with 83 and 69 publications in 2014 and 2015 respec-
tively, or packaging with 99 and 77 publications in 2014 and 2015
respectively as can be observed in Fig. 1.
Patent applications on nanocellulose include composite mate-
rials (38%), non-woven absorbent webs (18%), paper and boards
(16%), food products (13%), paper and board coatings (8%), cos-
metics and toiletries (3%), and filter materials (4%) (Koskinen,
Qvintus, Ritschkoff, Tammelin, & Pere, 2013; Tammelin et al.,
2013). Nanocellulose in the food industry can be used to develop
food packaging materials or food additives. However, most publi-
cations to date have been related to food packaging or additives to
Fig. 1. Number of publications per topic of interest among 733 publications related to nanocellulose (2006e2015 (October)).
Source: Scopus, VantagePoint, 2015. Search criteria: The words mentioned in Fig. 1 were searched using Scopus and VantagePoint. Each word must not be separated by more than
two words from the word “nanocellulose.”
179
polymer matrices as observed in Fig. 1. The paper published by
Turbak and co-workers in 1983 (Turbak et al., 1983a) was the first
scientific consideration of nanocellulose as a food additive; how-
ever, the product was not marketed owing to the high energy
consumption and production costs (Stro €
€ m, Ohgren, & Ankerfors,
2013). Currently, the isolation methods to produce nanocellulose
are more cost efficient, changing the perspectives on the industrial
production of the nanopolymer (Stro € m et al., 2013). This develop-
ment has enabled its availability as a commercial product, manu-
factured by various companies such as Daicel and Nippon paper in
Japan, Rettenmaier in Germany and UPM Kymmene and CelluForce
Co. in Canada (Charreau, Forestí, & Vazquez, 2013). Some research
institutes such as VTT in Finland and Innventia AB in Sweden have
also developed pilot plants to produce nanocellulose as a com-
mercial product (Charreau et al., 2013).
This paper aims to review the impact, benefits and challenges of
the use of vegetable nanocellulose in the food industry. Therefore,
relevant publications on the potential of nanocellulose in various
food applications were studied, focusing on publications about its
use as a food additive and safety and regulatory issues (Andrade
et al., 2015; Cunha, Mougel, Cathala, Berglund, & Capron, 2014;
Pitka€nen et al., 2010; Stro€m et al., 2013; Turbak et al., 1983a;
Winuprasith & Suphantharika, 2013, 2015). Reviews of nano-
cellulose as an additive in plastics to develop food packaging (Li,
Mascheroni, & Piergiovanni, 2015) or bacterial nanocellulose as a
food additive (Shi, Zhang, Phillips, & Yang, 2014) were found in the
literature. However, reviews of vegetable nanocellulose as food
additive were not found in the literature.
The literature review revealed the applications of vegetable
nanocellulose as a food stabilizer, functional food ingredient and
new packaging material in the food industry. However, the litera-
ture reports few validated standards to characterize the
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mez H. et al. / Food Hydrocolloids 57 (2016) 178e186
C. Go
nanostructure and evaluate the toxicity of nanomaterials in com-
plex matricesdfor instance, food matrices (La €htinen et al., 2012;
Szakal et al., 2014). To overcome these limitations and identify
real toxicity issues, it is important to understand changes intro-
duced in food matrices when interacting with nanocellulose during
preparation, storage and digestion (La €htinen et al., 2012; Szakal
et al., 2014). Therefore, this work also studied complementary
patents and publications related to the understanding of how
nanocellulose interacts with food matrices to fulfill the role of a
stabilizer or functional food ingredient.
2. Vegetable nanocellulose
Cellulose is a structural component in wood, cotton, natural fi-
bers and lignocellulosic materials. It represents approximately
1  1012 tons of the total annual biomass production (Hon, 1994;
Klemm, Heublein, Fink, & Bohn, 2005). Cellulose was discovered
by Payen in 1838, but it was previously used in the form of wood,
cotton, and other plant fibers as an energy source, building mate-
rial, and clothing (Klemm et al., 2011, 2005). Most of the important
developments to understand its chemistry and structure took place
between 1920 and 1940 (Klemm et al., 2011, 2005). The elucidation
of the polymeric structure of cellulose can be traced back to 1920
and the pioneering work of Staudinger (Hon, 1994; Klemm et al.,
2011). In the 1970s, the oil crisis generated considerable interest
in the use of cellulose as a source of biomass for the bioproduction
of organic chemicals (Fukuzumi, 2012). However, it was only in
1977 when researchers at the ITT Rayonier Eastern Research Divi-
sion Lab in Whippany, USA used a high-pressure Manton Gaulin
Milk Homogenizer to fibrillate a 3 wt% slurry of chopped pulp fi-
bers. They deconstructed the hierarchical structure of fibers,
obtaining considerable quantities of nanocellulose (Turbak et al.,
1983a). The first scientific article on this topic was presented at
the Ninth Cellulose Conference in 1981 and was later published in
the conference proceedings in 1983 (Turbak et al., 1983a).
The term “nanocellulose” is widely used to describe a range of
quite different cellulose-based nanomaterials that have one
dimension in the nanometer range such as whiskers, micro-
fibrillated cellulose, nanofibrillated cellulose and cellulose nano-
fibrils or microfibrils (Klemm et al., 2011; Stro €m et al., 2013).
However, in recent years, both the Technical Association of the Pulp
and Paper Industry (TAPPI) and the International Organization for
Standardization (ISO) have proposed standardization of the ter-
minology (Standard Terms and Their Definition for Cellulose
Nanomaterial WI 3021) and use the term “nanocellulose” only for
nano-scaled fibrils (TAPPI, 2011). In this work, the term “nano-
cellulose” is used for nano-scaled fibrils isolated from plants or
vegetal sources.
Isolation processes, characterization, and the search for appli-
cations of novel forms of cellulose nanomaterials, such as nano-
crystals or nanowhiskers and nanocellulose, have generated
significant interest in the scientific and industrial fields. Both
nanowhiskers and nanocellulose are cellulose-based nanomaterials
that can be isolated from vegetable sources via top-down and
bottom-up methods. Top-down methods include enzymatic/
chemical/mechanical treatments for their isolation from lignocel-
lulosic residues, whereas bottom-up methods involve production
of nanocellulose from glucose by bacteria (Castro et al., 2011;
Klemm et al., 2011). Nanowhiskers are needlelike cellulose crys-
tals 10e20 nm in width and several hundred nanometers in length
produced by strong acid hydrolysis to remove non-cellulosic
components and most amorphous cellulose from the source ma-
terials. Therefore, high-purity and crystalline cellulose nano-
material is produced.
Nanocellulose is a biopolymer made of repeating units of D-
glucoanhydropyranose linked by an ester bond b1/4. It is syn-
thesized by bacteria (Castro et al., 2011), algae (Horikawa &
Sugiyama, 2009), tunicates (Iwamoto, Kai, Isogai, & Iwata, 2009)
and plants (Zuluaga et al., 2009). Plants are the most abundant
source of cellulose (Moon, Martini, Nairn, Simonsen, & Youngblood,
2011). It is produced by a hexagonal array called rosette, generating
a nanofibril structure in the cell wall, in the presence of hemicel-
lulose and lignin. These non-cellulosic compounds help withstand
and transfer the loads exerted on the plant (Diotallevi, 2007;
Sturcova
, His, Apperley, Sugiyama, & Jarvis, 2004). Hydrogen
bonds and Van der Waals forces between the neighboring nano-
fibrils agglomerate them, forming the hierarchical structure of the
cellulose fiber (Parthasarathi et al., 2011).
Therefore, to develop products with vegetable nanocellulose, it
must first be chemically isolated. Several processes are used to
extract highly purified nanocellulose from the cell wall (Klemm
et al., 2011). They are generally based on successive chemical
treatments with alkaline solutions at different concentrations
(Zuluaga et al., 2009). Chemical treatments are followed by a me-
chanical treatment, which would break the side aggregations,
allowing a massive release of nanocellulose with diameters be-
tween 5 and 20 nm (Abe, Iwamoto, & Yano, 2007; Turbak et al.,
1983a). The most common mechanical techniques used are high-
pressure homogenization (Turbak et al., 1983a), microfluidizer
(Lavoine, Desloges, Dufresne, & Bras, 2012) waring blender (Uetani
& Yano, 2011; Zuluaga et al., 2009) and grinder (Abe et al., 2007).
Photographs of nanocellulose at different stages of the isolation
process can be observed in Fig. 2aeb. In addition, typical structures
of nanocellulose extracted from banana rachis by chemical
(Zuluaga et al., 2009) and mechanical treatments (high-pressure
homogenization at 500 bar), with diameters between 10 and 60 nm
are shown in the transmission electron microscopy (TEM) image
presented in Fig. 2c. Another well-known chemical pretreatment
employed in the manufacture of nanocellulose is TEMPO (2,2,6,6-
tetramethylpiperidine-1-oxyl)-mediated oxidation. In this pre-
treatment, the surface charge of nanofibrils is increased by oxida-
tion, and a slight mechanical treatment is then used to separate
them (Isogai, Saito, & Fukuzumi, 2011).
Isolated nanocellulose has significant large surface areas and
aspect ratios; therefore, its properties are sometimes significantly
different from those of the bulk materials (Fukuzumi, 2012).
Properties such as crystallinity, tensile strength, elastic
modulus (214 MPa and 13.2 GPa for nanocellulose with an average
degree of polymerization of 1100) (Henriksson, Berglund, Isaksson,
Lindstro€m, & Nishino, 2008), dimensional stability, thermal sta-
bility (between 220
C and 350
C) (Fukuzumi, 2012) and chemical
functionality (e.g., for modification) make nanocellulose a versatile
material with multifunctional properties with a wide range of ap-
plications as a food additive.
3. Vegetable nanocellulose in food applications
In the 1980s, Turbak and co-workers first proposed a list of
applications for nanocellulose as a food additive (Turbak, Snyder, &
Sandberg, 1982; Turbak et al., 1983a; Turbak, Snyder, & Sandberg,
1983b, 1984). In a series of scientific publications and patents,
they demonstrated that nanocellulose tends to stabilize oil-in-
water (o/w) emulsions because it is wet better by water than oil.
It is an excellent suspending medium for other solids and an
emulsifying base for organic liquids. For example, oil/water emul-
sions containing up to 71.5 wt% oil were stabilized by adding be-
tween 0.25 and 2.00 wt% of nanocellulose. Therefore, nanocellulose
can be used to stabilize oils or fats in foods (Turbak et al., 1982,
1983b). It has wide utility in the preparation of whipped toppings
(Turbak et al., 1982, 1983a), cake frostings (Turbak et al., 1983a),

mez H. et al. / Food Hydrocolloids 57 (2016) 178e186
C. Go 181

Fig. 2. Photographs of nanocellulose from banana rachis at different stages of the isolation process (a) nanocellulose after chemical treatments (b) nanocellulose after mechanical
treatments (c) TEM image of isolated nanocellulose.

Fig. 3. Nanocellulose properties to develop food application.

salad dressings (Turbak et al., 1983a, 1983b, 1984), gravies (Turbak
et al., 1982, 1983a), and sauces (Turbak et al., 1982, 1983a, 1983b).
During the same decade, other companies such as the Japanese
company Daicel, Procter & Gamble and Asahi Foods Co., Ltd. were
also very active in publishing on nanocellulose as food additive.
They used nanocellulose as a stabilizing agent in bean jam
(Mizuguchi, Fujioka, & Kobayashi, 1983a), sauce and soy soup
(Mizuguchi, Fujioka, & Kobayashi, 1983b), retort food (Mizuguchi,
Fujioka, & Kobayashi, 1983c), dough-based products (Koh &
Hayama, 1997), and whipping cream (Koh & Hayama, 1997). An
invention using nanocellulose as a functional food ingredient was
also developed. Daicel Chemical Industries developed a food or
drug for treatment of intestinal disorders using nanocellulose and a
water-soluble saccharide (Innami & Fukui, 1987).
Other incremental publications on the subject of nanocellulose
as a food additive subsequently appeared until 2013. These publi-
cations used the work of Turbak and co-workers to study in depth
the utility of cellulose as a food additive. The mechanism by which
nanocellulose stabilizes emulsion has been explained by means of
scanning electron microscopy or transmission electronic micro-
scopy and confocal laser scanning microscopy (Cunha et al., 2014;
Winuprasith & Suphantharika, 2013). Dispersed nanocellulose is
adsorbed at the oilewater interface to form steric barriers around
the emulsion droplets, which prevents their coalescence (Cunha
et al., 2014; Winuprasith & Suphantharika, 2013, 2015). Another
recent publication patented the use of nanocellulose to improve the
shape retention of frozen dessert and increase the time until
melting and falling (Yano, Abe, Kase, Kikkawa, & Onishi, 2012). The
most recent publication evaluated the improvement in the
healthiness to consumers, safety aspects and side effects of nano-
cellulose as dietary fiber. The results of animal trials carried out
with mice under a controlled diet prepared using different amounts
nanocellulose are reported (Andrade et al., 2015).
A gap in scientific publications and patents between the 1980s
and the last decade was identified. The first batch of scientific
publications and patents on nanocellulose as a food additive started
with Turbak and co-workers. The second batch started in the last
decade, triggered by worldwide interest in nanotechnology
(Charreau et al., 2013) and by improvements in nanocellulose
production that allow its commercialization. The most relevant
results and publications on nanocellulose as a food additive are
subsequently discussed. Uses of nanocellulose to develop food
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C. Go

packaging were also studied.
Moreover, scientific publications on the characterization of
nanocellulose have allowed several physicochemical properties to
be identified, some of which are very useful to develop new food-
related applications for nanocellulose (Klemm et al., 2005). Fig. 3
shows some properties of nanocellulose that are useful for appli-
cation in the food industry. For example, following the gray lines in
the diagram, it is observed that the high surface area and aspect
ratio, along with the rheological behavior and water absorption, are
very useful properties when using nanocellulose as a stabilizing
agent in food.
3.1. Nanocellulose as a food stabilizer
Nanocellulose as a natural emulsifying and stabilizing ingre-
dient is of great interest in food products such as salad dressings,
whipped toppings, sauces, foams, soups, puddings, dips, and many
others (Mizuguchi et al., 1983a, 1983b, 1983c; Turbak, Snyder, &
Sandberg, 1984; Winuprasith & Suphantharika, 2015). In 2013,
the report “nanocellulose as an additive in foodstuff” was published
in cooperation between the Swedish Institute for Food and
Biotechnology (SIK) and Innventia AB. In this report, the authors
concluded that nanocellulose has interesting potential as a stabi-
lizing agent for emulsions (Stro € m et al., 2013). Several scientific
publications and patents have been developed in this field (Cunha
et al., 2014; Stro € m et al., 2013; Turbak et al., 1982, 1983b;
Winuprasith & Suphantharika, 2013, 2015). Table 1 summarizes
some of the patents that use nanocellulose as an additive to
enhance the homogeneity and/or stability of a wide variety of
foodstuffs. In the cases studied, cellulose compared to the products
which it replaces, like fat base cream fillings, brings similar
organoleptic properties such as consistency and unctuousness
(Kleinschmidt, Roberts, Fuqua, & Melchion, 1988). Nanocellulose
also replaces stabilizers and emulsifiers like hydrophilic poly-
saccharides extracted from seaweed, vegetable seeds, microor-
ganisms or the like; insoluble polysaccharides such as
microcrystalline cellulose; and synthetic stabilizers such as
carboxymethylcellulose (Yano et al., 2012). Several advantages for
using nanocellulose as a stabilizer have been investigated.
Turbak and co-workers identified cost savings in preparing the
nanocellulose and the suspension in a single-stage operation. They
formed the nanocellulose in situ in the suspension by mixing
fibrous cellulose with the ingredients of the suspension and then
passing the mixture through a homogenizer (Turbak et al., 1982,
1983b). In some cases, suspensions may be made that were not
previously possible. For example, small amounts of nanocellulose
(0.94 wt%) are able to stabilize emulsions with soybean oil up to
71.5 wt%. Emulsions were not made with lower nanocellulose
content (Turbak et al., 1982).
The most recent patent of nanocellulose as a stabilizer was
developed by Yano and co-workers in 2014 (Yano et al., 2012). The
patent used nanocellulose to increase the period of time in which a
frozen dessert can retain its shape. The improvement in the shape
retention with stabilizers can be achieved by increasing the amount
of stabilizers. However, the addition of high amounts makes the
texture pasty and significantly impairs the flavor of the frozen
dessert. Adding between 0.10 and 0.30 wt% of vegetable nano-
cellulose extended the shape retention time without adversely
affecting the other properties. In all cases, nanocellulose increased
the time before the product melted and fell. A major improvement
was achieved in a hard ice cream with 0.30 wt% of nanocellulose.
The time before melting and falling was increased from 230 5200 to
350 2500 . Because of the small quantity of nanocellulose, it was un-
necessary to change the composition of the dessert mix, so good
flavor and texture could be achieved, and the properties of the
frozen dessert were not adversely affected when the shape reten-
tion was improved (Yano et al., 2012).
A number of publications tend to explain why cellulose can act
as a stabilizer. Emulsions can be formed and stabilized not only by
surface-active compounds, such as surfactants or proteins, but also
by solid particles to form “Pickering emulsions” (Pickering, 1907).
These emulsions mostly refer to the use of inorganic particles as
emulsifiers, including silica (Andrade et al., 2015; Cunha et al.,
2014), calcium carbonate (Andrade et al., 2015; Cunha et al.,
2014), montmorillonite (Andrade et al., 2015; Cunha et al., 2014),
and others. The particles accumulate at the oilewater interface to

Table 1
Summary of patents that use nanocellulose as an additive to enhance the homogeneity and stability of food.

Title Description

Food products containing microfibrillated Nanocellulose was prepared in situ during preparation of the food product to form a stable homogeneous suspension.
cellulose US 4341807 This process is useful for producing fillings, crushes, soups, gravies, puddings, dips, toppings and other food products.
The process has cost advantage of preparing the nanocellulose and food product in a single-stage operation (Turbak
et al., 1982).
Suspensions containing microfibrillated cellulose It was discovered that nanocellulose has the unique capability to enhance the homogeneity and stability of a wide
US 4378381 variety of suspensions. The presence of nanocellulose in suspensions of the type used in foods, cosmetics,
pharmaceuticals and industrial products such as paints and drilling muds has been found to confer a number of
unusual characteristics on the resulting product. In some cases, suspensions may be made that were not previously
possible (Turbak, Snyder, & Sandberg, 1983a,b).
A Liquid or pasty seasoning composition A sauce and soy soup with a necessary thixotropic property and storage stability were prepared by adding an
JP58190369 extremely small amount of nanocellulose as an additive (0.02e0.7 wt%) (Mizuguchi et al., 1983b).
Bean jam or food composition prepared by using A bean jam was prepared by adding 0.005e0.5 wt% of nanocellulose. The nanocellulose has a high binding property to
the same JP58190352 water and is easily dispersible finely in water. Therefore, the physical properties of the resultant product can be
improved by adding a small amount of nanocellulose to the raw bean jam and the high water retaining property.
Crispiness and fine touch to the mouth were obtained without changing the amount of sugar to be added (Mizuguchi
et al., 1983a).
Preparation of retort food JP58190382 A retort food was blended with 0.02e0.7wt% water dispersion of nanocellulose, based on the amount of the fluidic part
of the food or the amount of water, and it was heat-treated under high pressure. Nanocellulose showed good
palatability when used in a water dispersion for food (Mizuguchi et al., 1983b).
Use of cellulose microfibrils in dry form in food The invention concerns the use, in dry form, of a combination of nanocellulose with at least a polyhydroxylated
formulations US 6485767 compound as an additive for food formulations. The amounts of nanocellulose, relative to the additive(s) that they
replace, are lower. Moreover, it was found that the dried, combined nanocellulose has very good texturizing
properties; i.e., it has a role as a stabilizer and thickener in the formulation into which it is introduced (Cantiani,
Knipper, & Vaslin, 2002).
Frozen dessert and frozen dessert raw material EP The invention improved the shape retention of frozen dessert by the addition of nanocellulose. No adverse effect on
2756762 A1 viscosity, texture or flavor was observed (Yano et al., 2012).

mez H. et al. / Food Hydrocolloids 57 (2016) 178e186
C. Go
form a physical (steric) barrier that protects the emulsion droplets
against coalescence. The steric barrier is more effective for adsor-
bed particles that are preferentially wetted by the continuous
phase and lie predominantly on the outer surface of the dispersed
droplets (Winuprasith & Suphantharika, 2013).
Bio-based particles from renewable resources such as nano-
cellulose are suitable options to develop Pickering emulsions. They
allow for the manufacture of environmentally friendly materials
and can provide a wide range of aspect ratios and lengths (Andrade
et al., 2015; Cunha et al., 2014). Very firm emulsions have been
developed using 1 wt% of nanocellulose and oil by means of high-
pressure homogenization. The nanocellulose improved its incor-
poration between the oil droplets under higher pressure
(1000 bar). Emulsions were characterized by confocal laser scan-
ning microscope (CLSM), indicating that oil droplets were incor-
porated in a network of nanocellulose fibers resulting in their steric
€m et al., 2013). Winuprasith and Suphantharika
stabilization (Stro
(Winuprasith & Suphantharika, 2013, 2015), proposed a similar
mechanism for the formation and stabilization of 10 wt% soybean
oil-in-water (o/w), with a nanocellulose concentration in the
aqueous phase that varied from 0.05 to 0.70 wt%. They suggested
based on scanning electron microscopy (SEM) and CLSM charac-
terization that the suspension formation and stabilization could be
caused by the adsorption of nanocellulose at the oilewater in-
terfaces, providing a steric barrier against droplet coalescence by
the Pickering mechanism.
In addition, double Pickering emulsions o/w/o have been
developed using a combination of two types of nano-
cellulosedchemical tailored and native, with average diameters of
8 ± 3 nmddetermined by transmission electron microscopy (TEM).
The chemical modification adopted in this approach involved the
partial esterification of the hydroxyl groups from cellulose with a
fatty acid chloridednamely, lauroyl chloride. The surface accessi-
bility/concentration of the modified nanocellulose proved to be a
crucial parameter in the stabilization of the double emulsions. The
o/w/o double emulsions presented remarkable stability over a
month with average globule diameter of 65 ± 27 mm (Cunha et al.,
2014).
Nanocellulose in dry form has also been used as a stabilizer in
food formulations (Cantiani et al., 2002). The authors identified that
it was also a thickener in the formulation and could legitimately at
least partially replace fats for the preparation of reduced-fat for-
mulations (Cantiani et al., 2002). Therefore, nanocellulose can also
be used to reduce the energy density of foods.
3.2. Nanocellulose as a functional food ingredient
The potential of nanocellulose to prepare reduced-fat formula-
tions was also identified by Turbak and co-workers. Their patent
(US 4378381) demonstrated that nanocellulose may be substituted
for oil to produce a low-calorie salad dressing (Turbak et al., 1983b).
They mixed vinegar, nanocellulose and an envelope of dried Italian
salad mix. A stable dispersion of the spices resulted. The color and
texture of the material very closely resembled an authentic Italian
dressing.
Another characteristic of nanocellulose is dietary fiber. Nano-
cellulose is a type of dietary fiber that plays a beneficial role in the
overall health of adults; according to Hipsley's proposal, “Dietary
fiber is the edible parts of plants or analogous carbohydrates that
are resistant to digestion and absorption in the human small in-
testine with complete or partial fermentation in the large intestine.
They include polysaccharides, oligosaccharides, lignin, and associ-
ated plant substances” (AACCdAmerican Association of Cereal
Chemists, 2001). It is well established that dietary fiber offers a
range of health benefits and can assist in reducing the risk of
183
chronic diseases such as diabetes, obesity, cardiovascular disease,
and diverticulitis. In addition, it promotes beneficial physiological
effects including laxation, blood cholesterol attenuation, and blood
glucose attenuation (Andrade et al., 2015; Shi et al., 2014). A patent
has described the use of nanocellulose to treat intestinal disorders.
The inventors developed dried foods and drugs (powdered)
comprising 15 to 65 wt% of nanocellulose and 85 to 35 wt% of a
water-soluble saccharide to prevent agglomeration of nano-
cellulose. The powdered material can be added to foodstuff and was
successfully used in treating intestinal disorders (Innami & Fukui,
1987).
The term “functional food ingredient” was first used in Japan in
1984 (Ohama, Ikeda, & Moriyama, 2008). Japanese government
refers to it as “food products fortified with special constituents that
possess advantageous physiological effects” (Martirosyan & Singh,
2015; Siro
, Ka
polna, Ka

polna, & Lugasi, 2008). These products in
Japan can also take the form of capsules and tablets (Ohama et al.,
2008).
Unlike Japan, the European Union and United States govern-
ments do not have a formal legislative definition for “functional
food ingredient”. This term has already been defined several times,
but until now there is no officially approved definition (Siro
et al.,
2008). However, international organizations have developed their
own definitions (Diplock et al., 1999; Martirosyan & Singh, 2015).
The European Commission's Concerted Action on Functional
Food Science in Europe (FuFoSE), coordinated by International Life
Science Institute (ILSI) defined functional food ingredient using the
following statement: ‘‘a food product can only be considered
functional if together with the basic nutritional impact it has
beneficial effects on one or more functions of the human organism
thus either improving the general and physical conditions or/and
decreasing the risk of the evolution of diseases. The amount of
intake and form of the functional food should be as it is normally
expected for dietary purposes’’ (Diplock et al., 1999; Siro
et al.,
2008).
The Food and Nutrition Board (FNB) of the National Academy of
Sciences in the US “use the term functional food ingredient to
encompass potentially healthful products. A functional food may
include any modified food or food ingredient that may provide a
health benefit beyond the traditional nutrients it contains”
(Thomas & Earl, 1994).
The Institute of Food Technologists (IFT) defines it as: “food
ingredientes and food components that provide a health benefit
beyond basic nutrition. These substances provide essential nutri-
ents often beyond quantities necessary for normal maintenance,
grow and development and/or other biologically active compo-
nents that impart health benefits or desirable physiological effects”
(Martirosyan & Singh, 2015).
The American Dietetic Association (ADA), calls functional food
ingredient “Whole, fortified, enriched or enhanced that should be
consumed regularly and at effective amounts in order to derive
health benefits” (Kruger & Mann, 2003; Martirosyan & Singh,
2015).
Finally, in 2012 the Functional Food Center (FFC) at the FFC's 10th
International Conference in Santa Barbara, CA, announced a new
proposed definition: “Natural or processed foods or food in-
gredients that contains known or unknown biologically-active
compounds; which in defined amounts provide a clinically
proven and documented health benefit for the prevention, man-
agement, or treatment of chronic disease” (Martirosyan & Singh,
2015).
Definitions of FNB, IFT and FFC are comparable to the FuFoSE
definition. They highlight the idea that functional food ingredient
improves health in addition to providing basic nutrition. According
to this, nanocellulose could be considered as a potential functional
184
mez H. et al. / Food Hydrocolloids 57 (2016) 178e186
C. Go

food ingredient. Because, its dietary fiber characteristic can be used
to treat intestinal disorders (Andrade et al., 2015; Innami & Fukui,
1987).
In addition, nanocellulose can be used to produce low calorie
foods to treat weight disorders (Cantiani et al., 2002; Robson, 2012;
Turbak et al., 1983b). Food technologists are producing functional
foods and functional food ingredients to help people meet dietary
recommendations (for example, to consume foods with fewer cal-
ories or less total fat, saturated fat, and cholesterol) (Kruger &
Mann, 2003). There is a relationship between the consumption of
an energy-dense diet and obesity; thus, low-energy-density diets
(<1.6 kcal/g) are recommended for weight management (Robson,
2012). Amorphous cellulose, which has a high water content, has
been used successfully to reduce fat levels and hence reduce the
energy density of cheese, hamburgers, baked goods and sausages.
Nanocellulose, with a higher water content than amorphous cel-
lulose, could also be used to reduce the energy density of many
processed foods (Robson, 2012). It was proposed by A. Robson, a
researcher of the Universit
e de Bretagne Occidentale in France, that
nanocellulose could be used to reduce the energy density of foods
such as chocolate (Robson, 2013). Nanocellulose has used as an
additive to lower the food energy density in hamburger (Stro €m
et al., 2013), toppings (Cantiani et al., 2002), and dough-based
products (Kleinschmidt et al., 1988) as shown in Table 2.
Low water activities (i.e., below 0.6) are often needed in baked
goods to keep them crisp and crunchy. Fat-based creme fillings can
be used, but fat typically accounts for approximately 33% of its
weight. Crisp and crunchy fruit-filled cookies with water activities
of 0.2 were developed by adding from 0.3 wt% to approximately
2 wt% of nanocellulose. Replacement of fat with nonfat ingredients
such as nanocellulose could reduce the calories of fillings by
15e20 wt% (Kleinschmidt et al., 1988).
3.3. Nanocellulose in food packaging
Historically, packages have been created with four basic func-
tions: protection, communication, convenience, and containment;
however, these functions are no longer sufficient because society is
becoming more exigent about food-related products (Silvestre,
Duraccio, & Cimmino, 2011). Material science, nanotechnology,
food engineering, biology and chemistry are working together to
develop a new generation of products with new and improved
properties. The idea behind the incorporation of nanotechnology in
packaging systems is to increase the shelf life and nutrition capacity
of food and communicate food quality to customers (Robinson &
Morrison, 2010). Currently, food packaging must be designed to
increase the shelf life or safety of the contained products. Antimi-
crobial agents and oxygen and moisture barriers are usually used in
packaging systems for food. Films made purely of nanocellulose
have a very high air and oxygen barrier. The oxygen permeability of
nanocellulose films with thickness of 21 ± 1 mm was
17 ± 1 ml m2 day1. This value makes nanocellulose competitive
with synthetic polymers such as ethylene vinyl alcohol (EVOH)
(3e5 ml m2 day1) and polyester-oriented, coated polyvinylidene
chloride (PVdC) films (9e15 ml m2 day1) of roughly the same
thickness (Nair, Zhu, Deng, & Ragauskas, 2014).
The excellent oxygen barrier properties of nanocellulose films
are due to a combination of a high crystallinity, a network structure
held together via strong inter- and intramolecular hydrogen bonds,
a lamellar nanofiber structure and dense fiber packing (Fukuzumi,
2012; Svagan et al., 2016). However, oxygen permeability of
nanocellulose films depends on relative humidity (RH). At low RH
(0 %), nanocellulose films show very low oxygen permeability
compared with films prepared from plasticized starch, whey pro-
tein and arabinoxylan, with oxygen permeability values in the same
range as conventional synthetic films, such as ethylene vinyl
alcohol. At higher RH's, the oxygen permeability increases expo-
nentially because of the plasticizing and swelling of the nano-
cellulose by water molecules (Aulin, G€ € m, 2010).
allstedt, & Lindstro
In addition, global environmental concern regarding the use of
petroleum-based packaging materials is encouraging researchers
and industries to search for packaging materials from natural bio-
polymers. However, applications of biopolymers in the packaging
industry are limited by their low mechanical properties and high
water and oxygen permeability due to the number of hydroxyl
groups present in its structure. Nanocellulose is used to increase
both mechanical properties and permeability properties of oxygen
(Aulin et al., 2010; Li et al., 2015; Nair et al., 2014; Svagan, Azizi
Samir, & Berglund, 2007; Syverud & Stenius, 2009). Fukuzumi
et al. (2011), prepared high-oxygen-barrier nanocellulose films by
TEMPO mediated oxidation. The 0.80 mm thick nanocellulose film,
when coated on a 25 mm polylactic acid film, reduced the oxygen
permeability from 7.4 ml m2 day1 kPa1 for pure a PLA film to
9.9  104 ml m2 day1 Pa1 for PLA film with a nanocellulose
layer. Although the oxygen barrier properties of nanocellulose films
are competitive with the currently available commercial films
made from synthetic polymers, their water vapor barrier remains
low mainly because of the strong hydrophilic nature of the nano-
cellulose (Nair et al., 2014). Several chemical treatments are avail-
able to increase water barrier properties (De Azeredo, 2009),
including acetylation, which creates a higher hydrophobic film
surface indicated by the increase in the contact angle with water
(Ashori, Babaee, Jonoobi, & Hamzeh, 2014; Forestí, Avila Ramirez,
Go
mez, Arroyo, & Cerrutti, 2016; Rodionova, Lenes, Eriksen, &
Gregersen, 2011).
4. Safety and regulatory issues of nanocellulose in food
Nanocellulose is an abundant and sustainable nanomaterial
with potential applications in the food industry. It improves the
performance of many products as discussed. However, it still ex-
hibits unknown properties and thus may expose humans and the
environment to unknown risks. Wood pulp and powdered cellulose
are generally recognized as being safe (GRAS) and can be used as a

Table 2
Nanocellulose as additive to reduce the energy density of foods.

Food Description Ref.

Hamburger Hamburgers had no off-flavor and had the same texture and mouth feel as the hamburger without nanocellulose. It held more € m et al., 2013).
(Stro
water without side effects as a watery taste, and it was easy to mix with the meat, but owing to its low dry weight, the proper
amount of nanocellulose was difficult to add without adding excessive water.
Toppings The patent US 6485767 mentioned that an additional advantage of nanocellulose use to stabilize food is that it represents only a (Cantiani et al.,
small supply of calories and can legitimately, totally or partially replace fats to prepare reduced-fat compositions. 2002)
Dough based Fruit-filled cookies with water activity near 0.2 without the formation of unwanted textures or the collapse of the baked product (Kleinschmidt et al.,
products and with a crispy and crunchy texture were developed by adding from 0.3 wt% to approximately 2 wt% of nanocellulose 1988)
(Kleinschmidt et al., 1988).

mez H. et al. / Food Hydrocolloids 57 (2016) 178e186
C. Go
raw material for food contact materials or even as food additives
(L€
ahtinen et al., 2012). However, in nanomaterials, the biological
impacts on ecosystems and humans cannot be evaluated merely on
their chemical characteristics. The size, shape, aggregation prop-
erties and different unknown factors might still affect the in-
teractions of nanocellulose with cells and other living organisms.
Studies supporting risk management have lagged far behind the
advancement of the technology (Szakal et al., 2014). Evidence
suggests that this growing knowledge gap is leading to a public
perception that there are more risks than benefits associated with
nanomaterials (Szakal et al., 2014). Currently, few in vitro and in vivo
studies have investigated the toxic properties of nanocellulose
(Andrade et al., 2015; Pitka€nen et al., 2010; Vartiainen et al., 2011).
€nen et al. (2010), assessed the in vitro cytotoxic and geno-
Pitka
toxic properties of nanocellulose made from birch pulp and grinded
once, with diameters between 20 and 60 nm, and with a large
fraction at 100e0.350 mm. Short-term toxicity (24e72 h exposures)
measured by the change in the total protein content in several
human or animal cell lines and sub-lethal effects were tested on
cultured human cells. The ability to damage DNA was assessed
using a bacteriological assay (Ames test). No indication of DNA
damage, based on the Ames test, was observed; therefore, toxico-
logical tests did not indicate any cyto- or genotoxic properties.
Another in vitro study on the toxic properties of nanocellulose
was developed by Vartiainen et al. (2011). They assessed the health
and environmental safety aspects of friction-grinded and spray-
dried nanocellulose with diameters between 20 and 30 nm. To
evaluate the health effects, mouse macrophages and human mac-
rophages were exposed to nanocellulose, and the viability and
cytokinetic profile of the cells were studied. No inflammatory effects
or cytotoxicity in mouse or human macrophages was observed after
6 and 24 h exposures to the materials. The results of the toxicity
studies suggested that nanocellulose is not cytotoxic and does not
have any effect on the inflammatory system in macrophages.
Recently, Andrade et al. (2015) developed an in vivo study in
which male mice (Rattus norvegicus albinus) were fed a diet that
contained 7 wt%, 14 wt% and 21 wt% nanocellulose suspension from
peach palm. The diets were prepared following the criteria used for
AIN-93 (Reeves, Nielsen, & Fahey, 1939). It was demonstrated that
this amount of nanocellulose did not cause harmful effects in the
animal metabolism, indicating that it could be used as a dietary
supplement (Andrade et al., 2015).
Therefore, different in vivo and in vitro tests have been used to
determine the toxicity of nanocellulose. According to the results of
the aforementioned research, nanocellulose does not create cyto-
toxic or genotoxic concerns. However, to obtain more unambiguous
information on the safety impacts of nanomaterials such as nano-
cellulose, internationally standardized methods are needed to
ensure their safety (La€htinen et al., 2012; Szakal et al., 2014). Before
food products using new nanotechnologies are commercialized,
there is a need to anticipate, understand, and manage the poten-
tially positive and negative effects that might result from nano-
material consumption (Szakal et al., 2014).
5. Conclusions
The potential of vegetable nanocellulose as a food additive was
first identified in the 1980s. Several investigations of nanocellulose
as a food additive were published and patented at that time.
However, only in the last decade have improvements in nano-
cellulose production allowed for its commercialization, which
again increased the number of publications.
According to these publications, nanocellulose creates a physical
(steric) barrier that protects the droplets in oil water emulsion
against coalescence because nanocellulose has better affinity with
185
water than with oil. Therefore, nanocellulose has very good poten-
tial as a stabilizing agent for emulsions and food. It could be used to
stabilize oils or fats in different types of foods, such as crushes,
soups, gravies, puddings, dips, toppings, frozen desserts and meats.
Stable emulsions with lower oil content can be produced using
nanocellulose, and nanocellulose may be substituted for oil in some
cases to produce low-calorie foods. Nanocellulose has been used to
reduce the caloric value of food. The replacement of fat with nonfat
ingredients such as nanocellulose could reduce the calories in fill-
ings by 15e20 wt%. Dietary fiber was another identified application
for nanocellulose as a food additive. The patent of a successful
formulation used for treating intestinal disorders was discussed.
The dietary fiber characteristic and utility to produce low-calorie
foods makes nanocellulose a functional food ingredient.
The potential of vegetable nanocellulose as a food has been
studied from several scientific aspects. However, a final step is still
required to achieve complete industrialization and incorporation of
nanocellulose in everyday life. Validated standards to characterize
the obtained nanostructure, quantify its properties and evaluate its
toxicity in complex matrices such as foods are required to avoid
uncertainties about its secondary or toxic effects in humans.
Acknowledgments
The authors acknowledge the Administrative Department of for
Science, technology and Innovation of the Colombian Government
(COLCIENCIAS) and the Research Center for Investigation and
Development (CIDI) from the Universidad Pontificia Bolivariana for
their financial support through the program Es tiempo de volver
(Grant 363B-02/15-49). The authors are also grateful to PhD J-L
Putaux from the Centre de Recherches sur les Macromol
ecules
V
eg

Joseph for the
etales (CERMAV-CNRS), affiliated with Universite
transmission electronic microscopy images (TEM). Finally the au-
thors are grateful to MSc. Ana Velasquez Giraldo for the support
with language and with the search and processing of information.
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