Carbohydrate Polymers 163 (2017) 301–316

Contents lists available at ScienceDirect

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

Review

Preparation, properties and applications of nanocellulosic materials

Subrata Mondal
Department of Mechanical Engineering, National Institute of Technical Teachers’ Training and Research (NITTTR), Salt Lake City, Kolkata, 700106, West
Bengal, India

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

Article history: Recently, nano materials derived from natural renewable resources have drawn much attention in the
Received 10 April 2016 nanotechnology research thrust. Lignocelluloses are composed of cellulosic nano-fibrils which can be
Received in revised form disintegrated by chemical, mechanical and enzymatic methods in order to obtain nanocellulose. Fur-
17 December 2016
ther, nanocellulose can also be synthesized by bacterial method in a suitable culture. Nanocelluloses
Accepted 20 December 2016
have many interesting properties (viz. nano-dimension, renewability, low toxicity, biocompatibility,
Available online 29 December 2016
bio-degradability, easy availability and low cost) which make them ideal nanomaterials for diverse appli-
cations. In this paper, author reviewed researches on recent advances in nanocellulosic materials. Various
Keywords:
Cellulose
methods of nanocellulose preparation and their properties, surface modifications of nanocellulose, and
Nanocrystal applications of nanocellulose in the diverse fields have been discussed in the paper.
Biomedical © 2016 Elsevier Ltd. All rights reserved.
Filler
Aerogel
Polymer nanocomposite

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 301
2. Various methods for the preparation of nanocellulosic materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 302
2.1. Mechanical methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 302
2.2. Chemical method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
2.3. Bacterial method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
3. Properties of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
4. Surface modification of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 304
5. Application of nanocellulosic materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
5.1. Biomedical applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 306
5.2. Energy, environmental and water related applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 307
5.3. Polymer nanocellulose nanocomposite . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 310
5.4. Other applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 311
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 312
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 312

petroleum based synthetic products due to their advantages of rel-

1. Introduction
atively low cost, environmental friendly in nature, easy availability,
renewability, and nontoxicity. Cellulose is the most abundant nat-
Novel materials derived from the low-cost and renewable
ural polymer in the planet Earth. By photo-synthesis processes,
resources have drawn significant interests to the materials sci-
plants synthesizes cellulose which accounts for approximately 40%
entists with the growing environmental concern of end-of-life
of lignocellulosic biomass (Mondal, Memmott, & Martin, 2014,
disposal challenges (Abraham et al., 2011). The materials obtained
Anirudhan, Gopal, & Rejeena, 2015; Abraham et al., 2011).
from the renewable bioresources could be the alternative of
Cellulosic nanofibrils are mainly composed of plant cell walls
and provide strength, toughness and stiffness to the plant anatomy.
Cellulosic nanofibrils in the form of nanocellulose can be extracted
E-mail address: subratamondal@yahoo.com from the lignocellulosic bioresources by using appropriate chem-

http://dx.doi.org/10.1016/j.carbpol.2016.12.050
0144-8617/© 2016 Elsevier Ltd. All rights reserved.
302 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316
Fig. 1. Number of publication with respect to the publication year based on nanocellulose (source: web of science; search key word (title): nanocellulose).
ical, mechanical, enzymatic or combination of more than one
method. Nanocellulosic material has been attracted considerable
research attention in recent years (Fig. 1) due its many exceptional
properties and potential for the diverse applications (Donius, Liu,
Berglund, & Wegst, 2014). Nanobiomaterials derived from abun-
dant and renewable natural resources could have the potential to
replace synthetic nanomaterials (Deepa et al., 2015). Nanocellulosic
materials have many interesting features such as nano dimension
(higher surface area to volume ratio), nontoxicity, biodegradability,
biocompatibility etc. Interesting properties of nanocellulose could
find applications in the biomedical field, reinforcement in polymer
matrix in order to fabricate nanocomposite, energy, environment
and so on so forth.
By definition, material that has at least one dimension less
than or equal to 100 nm, could be considered as nanomate-
rial (Espino-Perez, Domenek, Belgacem, Sillard, & Bras, 2014).
Nanomaterials derived from renewable cellulosic and lignocellu-
losic biomass could play a significant role in the nanotechnology
research domain (Gardner, Oporto, Mills, & Samir, 2008; Milanez,
do Amaral, Lopes de Faria, & Rodrigues Gregolin, 2013; Milanez
et al., 2014). Owing to the hierarchical structure of cellulose
molecules in the lignocellulosic biomass, nanocellulose can be
extracted by using an appropriate extraction methods (Dufresne,
2013). Various types of plant biomasses can be used to extract
nanosized cellulose, and the yield of nanocellulose could depends
on the source of lignocellulosic biomass, when same method of
extraction would be employed (Deepa et al., 2015). Advances of
nanotechnology research encourage scientists to develop nano-
materials from renewable bio-resources which have significantly
lowered environmental impact. Therefore, in this review paper,
author attempted to review the extraction of nanocellulose from
various lignocellulosic biomasses, surface modification of nanocel-
lulose, the characterization of nanocellulose and their potential
applications in the diverse fields.
2. Various methods for the preparation of nanocellulosic
materials
Nanocelluloses are accounted for various types of cellulosic
nanomaterials with at least one of its dimensions is less than or
equal to 100 nm by the definition of nanomaterials. Typical exam-
ples of nanocelluloses are cellulose nanofibrils (CNFs), cellulose
nanocrystals (CNCs) and bacterial nanocellulose (BNC) (Aitomaki
& Oksman, 2014; Charreau, Foresti, & Vazquez, 2013, Jorfi & Foster,
2015; Plackett, Letchford, Jackson, & Burt, 2014; Lin & Dufresne
2014). Nanocellulose can be extracted from various lingocellulosic
plant resources (Chen, Wu, Huang, Huang, & Ai, 2015; Chen, Xu,
Liu, & Zeng, 2015) by using mechanical, chemical or enzymatic
methods. Lignocellulosic biomass is a complex biomaterials which
consists of cellulose, hemicellulose, and lignin. Cellulose in the
lignocellulosic biomass can be disintegrated to nano dimension
materials by using appropriate methods (Lee, Hamid, & Zain, 2014).
Macro or micro structure of cellulose consists of amorphous as
well as crystalline phases. It is relatively easy to break the amor-
phous phase of cellulosic biopolymer by mechanical, chemical or
enzymatic means, while, it is quite difficult to break the nanostruc-
tured crystalline phase of cellulose due to the presence of enormous
hydrogen bonding. Extraction of nanocellulose from the cellulosic
biomass includes two major steps viz. pretreatment and removal
of amorphous phase by appropriate methods (Kim et al., 2015).
Prior to the mechanical, chemical or enzymatic treatment, pre-
treatments such as alkali treatment and bleaching are required.
The prime objective of pretreatment is to remove certain amount
of lignin, hemicellulose, wax and oils which cover on the exter-
nal surface of the fibre cell wall. Alkali treatment depolymerises
the native cellulose structure, defibrillates the external cellulose
microfibrils and exposes short length crystallites. Further, bleach-
ing treatment is required in order to remove the cementing material
completely from the fiber (Abraham et al., 2011). Nano dimensions,
quality and yield of nanocellulose would depend on source of lig-
nicellulosic biomass when same method of extraction is applied.
Abraham et al. reported nanocellulosic materials extracted from
three different lignocellulosic biomasses such as banana (pseudo
stem), jute (stem) and pineapple leaf fibre by pretreatment with
alkali followed by steam explosion and finally acid hydrolysis. The
quality and yields of nanocellulose derived from pineapple biomass
is better than the nanocellulose extracted from banana and jute
stem (Abraham et al., 2011). Apart from cellulose nanocrystal and
cellulose nanofibers, nano size bacterial nanocellulose (BNC) can be
synthesized by certain strains of bacteria in a favorable condition
(Aitomaki & Oksman, 2014).
2.1. Mechanical methods
Nanocellulose can be obtained by disintegrating cellulose
from the lignocellulosic biomass by mechanical means (Hettrich,
Pinnow, Volkert, Passauer, & Fische, 2014). Cherian et al. reported
acid coupled steam treatment method for the preparation of
nanocellulose from pineapple leaf fiber (Cherian et al., 2010).
The surface morphology of biomass changes with the removal of
primary components (Fig. 2). Pretreatment of biomass at high tem-
perature steam explosion with alkali hydrolyzes hemicellulose and
depolymerizes the lignin. Further, lignin is rapidly oxidized by chlo-
rine and accelerate the degradation of lignin. Formation of various
 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316 303

Fig. 2. Scanning electron microscopy (SEM) images of (a and b) raw chemical-thermomechanical pulps (CTMP); (c and d) fibers after acidified sodium chlorite treatment
(Ho-CFs); (e and f) fibers after alkali-treated (Al-CFs); and (g and h) NCFs (Li et al., 2014) [Reproduced with permission, Copyright © 2014 Elsevier Ltd. All rights reserved].

groups such as hydroxyl, carbonyl and carboxylic groups facilitates
the lignin solubilization in the alkaline medium. Acid coupled steam
treatment helps to disintegrate fibrils to form the nanocellulose
(Cherian et al., 2010). Hettrich et al. reported a combined chemical
and mechanical method for the preparation nanocellulose by using
various cellulosic bioresources such as bleached pulp, cotton linters
and microcrystalline cellulose. Prior to the mechanical treatment,
pretreatments such as grinding, acid hydrolysis, decrystallization
and derivatization are used for the preparation of nanocellulosic
materials. Extracted cellulose has spherical shape with diameter of
304 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316

less than 200 nm (Hettrich et al., 2014). Jiang and Hsieh reported a mechanical properties and flexibility (Taokaew, Seetabhawang,
method for the cellulose nanofibrils preparation by using mechan- Siripong, & Phisalaphong, 2013; Iguchi, Yamanaka, & Budhiono,
ical defibrillation of rice straw using a high speed blender in three 2000; Chen et al., 2009). Biomaterial grade bacterial nanocellulose
consecutive blending and separation steps (Jiang & Hsieh, 2013). (BNC) could be synthesized by aerobic cultivation of the bacterium
Nanocellulose can be derived from the lingocellulosic biomass by Gluconacetobacter xylinus (synonym Komagataeibacter xylinus)
high pressure homogenization. The biomass could be suspended by in a glucose enriched medium (Ahrem et al., 2014; Gatenholm &
high speed stirring coupled with ultrasonication treatment prior Klemm, 2010; Feldmann et al., 2013; Fu, Zhou, Zhang, & Yang, 2013;
to the high pressure homogenization (Wang, Zhang, Jiang, Li, & Kubiak et al., 2014). Aramwit and Bang reported method of bacterial
Yu, 2015). Ionic liquid can be used to treat the lignocellulosic nanocellulose preparation by using the coconut water at suitable
biomass prior to the mechanical treatment. The ionic liquid per- culture media by a gram negative rod shaped bacterium, G. xylinus
meates through the microstructure of cellulose and subsequently, (Aramwit & Bang, 2014).
attacks the hydrogen bonds between cellulose molecules. During
high pressure homogenization, inter and intra molecular bonds are
3. Properties of nanocellulose
further destroyed, hence, nanocellulose is disintegrate from the
biomass. Extracted nanocellulose has a width of 10–20 nm (Li et al.,
Morphological structure of nanocellouse is highly dependent on
2012; Wang, Wei et al., 2015).
the efficient removal of non cellulosic part and dissolution of amor-
phous region of domain structure (Cherian et al., 2010; Lu et al.,
2.2. Chemical method
2013). Morphology (Table 1), physical property and dimension of
the nanocelluloses are varied significantly with the different natu-
Acid hydrolysis is a common method to extract nanocelluose
ral fiber resources and with the extraction processes. Deepa et al.
from the lignocellulosic biomass (Lin, Bruzzese, & Dufresne, 2012;
reported the morphology of nanocelluloses which were extracted
Lu et al., 2013; Saraiva Morais et al., 2013; Yongvanich, 2015;
by acid hydrolysis from sisal, pineapple leaf and coir; the nanofiber
Moran, Alvarez, Cyras, & Vazquez, 2008; Mandal & Chakrabarty,
shows long, flexible and entangled morphology, whereas, more
2011). After the hemicellulose removal and prior to the acid hydrol-
individualized and rod like structures (Fig. 3) are visible when
ysis treatment, the lignocellulosic biomass can be treated with
nanocelluloses are extracted from the banana rachis and kapok
chemical such as dimethyl sulfoxide to swell the matrix of biomass
(Deepa et al., 2015).
so that acid could diffuse into the domain structure of lignocellu-
Mechanical properties of the nanocellulose are better than their
losic biomass easily and disintegrate the nanowhisker (Mandal &
lingocellulosic source biomass materials because of more uniform
Chakrabarty, 2011). In an acid treatment method, yield of nanocel-
morphological structure. The average modulus of nanocellulose is
lulose depends on the content of lignocellulosic biomass and the
100 GPa which is much higher than the base celluloseic materi-
reaction conditions such as acid concentration, time and temper-
als (Dufresne, 2013). Crystal structure and degree of crystallinity
ature. Optimization of experimental parameters are required to
of the nanocellulose depends on the lignocellulosic resources (Le
obtain maximum yield and to preserve the nanocellulose mor-
Bras, Stromme, & Mihranyan, 2015). Nnanocellulose contain both
phology (Lu et al., 2013). Yield as well as nano dimension of
cellulose I and cellulose II, which could be characterized by typi-
nanocellulose decreases with the increase of acid treatment time
cal X-ray diffraction peaks at around 2(␪) ∼23◦ and 2(theta) ∼ 34◦
of cellulosic biomass (Shahabi-Ghahafarrokhi, Khodaiyan, Mousavi,
respectively (Peng et al., 2013).
& Yousefi, 2015). Preparation of nanocellulose from the lignocellu-
Thermal degradation property of nanocellulose depends on
losic biomass by using catalysts could be a green approach. Ionic
extraction procedure and source of cellulose bio-resources. In
liquid based catalyst has several advantages viz. wide range of
general, nanocellulose obtained from extracting natural cellulosic
electrochemical stability, good electrical conductivity, high ionic
resources have better thermal stability than the ␣-cellulose present
mobility, selective dissolution properties to many organic and
in the original lignocellulosic biomass (Abraham et al., 2011).
inorganic substances as well as excellent chemical and thermal
Improved thermal stability of nanocellulosic materials as compared
stabilities (Abd Hamid, Al Amin, & Ali, 2014). Ultrasound has signif-
to their source cellulose is due to their higher crystallinity, flexible
icant influence on nanocellulose property prepared from bleached
structure and removal of low thermal stable lignin materials (Deepa
hardwood kraft pulp oxidized by 2,2,6,6-tetramethylpiperidine-1-
et al., 2015).
oxyl (TEMPO). Nanocellulose prepared by using ultrasound assisted
Carboxylic functional group (189–1181 mmol/kg) containing
process is thinner, contain more carboxylic functionality, higher
nanocellulose gel shows shear thinning rheological behaviors.
degree of fibrillation, and higher yield (Mishra, Manent, Chabot, &
Therefore, with the increase of shear rate, nanocellulosic gel net-
Daneault, 2012; Mishra, Thirree, Manent, Chabot & Daneault, 2011;
work slowly broke up into individual entities, hence, reduces the
Mueller et al., 2013; Loranger et al., 2012). Satyamurthy and Vig-
final viscosity of the gels (Loranger et al., 2012; Loranger et al.,
neshwaran proposed a novel method of nanocellulose preparation
2013). Surface property of the nanocellulose would affect the shear
in an anaerobic microbial consortium for the controlled hydroly-
thinning rheology of the suspension (Rees et al., 2015).
sis of microcrystalline cellulose which was obtained from cotton
fibers. The advantages of this method are less energy consumption
due to enzyme (cellulase) assisted catalysis, no surface sulfation, 4. Surface modification of nanocellulose
preserve the chemical structure of cellulose, biocompatible as well
as potential to scale up (Satyamurthy & Vigneshwaran, 2013). Bulk applications of nanocellulose are often hindered due to the
poor dispersibility of nanocellulose in nonpolar organic solvent,
2.3. Bacterial method and nonpolar polymer matrix (in order to prepare the nanocom-
posite) (Kovalenko, 2014). Cellulosic nanofiller has a tendency to
Nanocellulose obtained by using bacterial method has similar aggregate due to the inter and intra molecular hydrogen bond-
chemical structure as with nanocellulose extracted from the ligno- ing between three hydroxyl groups of the repeat unit, and this
cellulosic biomass by following chemical and mechanical methods. results in poor dispersion of nanofillers in non polar solvent and non
In addition to this, ultrafine nanofiber network formed by an appro- polar polymer matrices. In order to utilize the nanofillers properly,
priate culture medium exhibits unique properties e.g. high purity, the fillers should be homogeneously dispersed and distribute in
uniform morphology, good water absorption capacity, excellent the matrices. Nanoscale dimension of nanocellulose has high spe-
 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316 305

Fig. 3. Transmission electron microscopy images showing the morphology of nanocellulose obtained from various sources a banana rachis b sisal c kapok d pineapple leaf
and e coir (Deepa et al., 2015) [Reproduced with permission, Copyright © 2015, Springer Science + Business Media Dordrecht].

Fig. 4. Various common chemical modifications approaches of nanocellulose [PEG: poly(ethylene glycol); PEO: poly(ethylene oxide); PLA: poly(lactic acid); PAA: poly(acrylic
acid); PNiPAAm: poly(N-isopropylacrylamide); and PDMAEMA: poly(N,N-dimethylaminoethyl methacrylate)] (Lin, Huang et al., 2012) [Reproduced with permission, Copy-
right © 2012, Royal Society of Chemistry].
306 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316

Table 1
Influence for the source of cellulosic biomass and preparation methods on the lateral dimension of nano-cellulose.

Source of cellulose Lateral dimension Preparation method References

Mengkuang leaves 5–25 nm Acid hydrolysis (El Sheltami et al., 2012)

(Pandanus tectorius)
Banana rachis 10–60 nm Acid hydrolysis (Deepa et al., 2015)
Sisal 20–80 nm Acid hydrolysis (Deepa et al., 2015)
Kapok 20–70 nm Acid hydrolysis (Deepa et al., 2015)
Pineapple leaf 50–150 nm Acid hydrolysis (Deepa et al., 2015)
Coir 40–90 nm Acid hydrolysis (Deepa et al., 2015)
Soft wood pulp 10–20 nm High shear defibrillator (Faruk et al., 2014)
Cladophora sp. green algae 30–40 nm Oxidation (Carlsson et al., 2014)
Cotton linters 39 ± 7 nm Acid hydrolysis (Carlsson et al., 2014)
Pineapple leaf fibre 5–60 nm Steam explosion acid hydrolysis (Cherian et al., 2010)
Microcrystalline cellulose 6.96 nm Acid hydrolysis (Cho & Park, 2011)
Cellulose powder 20–50 nm High-pressure homogenizer (Chun et al., 2012)
Leaves licuri 5.7–61.6 nm Acid hydrolysis (Costa et al., 2014)
Kraft bagasse pulp 7.5–16.5 nm Acid hydrolysis (El-Wakil et al., 2015)
Gluconacetobacter xylinus 128 nm Bacterial synthesis (Heßler & Klemm, 2009)
spruce and pine 5–10 nm Acid hydrolysis (Ishikawa et al., 2015)
Rice straw 1.5–12.6 nm High speed blender (Jiang & Hsieh, 2013)
Rice straw 1.4–8.5 nm Acid hydrolysis (Jiang & Hsieh, 2013)
Rice straw 1.73 ± 0.56 TEMPOa oxidation (Jiang & Hsieh, 2013)
Bamboo fiber 10–30 nm Alkali and acid hydrolysis (Jiang, Zhang et al., 2015)
Rice straw 40–80 nm Acid hydrolysis (Kardam et al., 2014)
Cotton lint <50 nm Acid and mechanical (Nahr et al., 2015)
Maize straw 15–25 nm Acid hydrolysis (Rehman et al., 2014)
Pomelo Fruit Fibers 10–20 nm Acid hydrolysis Yongvanich 2015)
Citrus waste 10 nm Enzymatic hydrolysis (Mariño et al., 2015)
a
TEMPO-2,2,6,6- tetramethylpiperidine-1-oxyl.

cific surface area which ensures plenty of hydroxyl groups on the
nanocellulose surfaces which could be used for the chemical mod-
ification of nanocellulose surface (Lin, Huang, & Dufresne, 2012).
Chemical modification should be mild to preserve the other useful
properties of nanocellulose. Chemical modification of nanocellu-
lose can be classified into three groups a) molecules grafting on
nanocellulose, b) molecules grafting to nanocellulose, b) substitu-
tion of hydroxyl groups with small molecules (Dufresne, 2013).
Various strategies of nanocellulose modifications are illustrated
schematically in Fig. 4.
Espino-Perez et al. proposed solvent free chemical modification
of nanocellulose with carboxylic groups. Appropriate functional
molecules could be attached with nanocellulose by SolReact
method by esterification of hydroxyl groups of nanocellulose with
carboxylic groups of aromatic carboxylic acids. The method has
several advantages such as less toxic carboxylic acid for graft-
ing, low reaction temperature, reaction at ambient pressure and
recycle of excess reactant by distillation technique (Espino-Perez
et al., 2014). Carboxylic functionalities could introduce into the
nanacellulose by oxidation method, and the carboxylic function-
alities could serve as templates to bind various biomolecules such
as fluorescent amino acids, peptides etc. Amino acid or peptide
can bind with oxidized nanocellulose by nucleophilic reaction
between the amine group (-NH2 ) and carboxylic group (Barazzouk
& Daneault, 2011; Barazzouk & Daneault, 2012a; Barazzouk &
Daneault, 2012b). In general, carboxylic functionalities are intro-
duced into the nanocellulose surfaces by carboxymethylation or
2,2,6,6- tetramethylpiperidine-1-oxyl (TEMPO) mediated oxida-
tion method (Carlsson, Lindh, Nyholm, Stromme, & Mihranyan,
2014).
Surface chemistry of nanocellulose can be engineered by
pretreatment of the raw nanocellulose fibres by using car-
boxymethylation and periodate oxidation methods. Pretreatment
introduces aldehyde and carboxyl groups on the nanocellulose sur-
face. Further, aldehyde and carboxylic functionalities could react
with other appropriate functional groups to form covalent bonding,
for an example, aldehyde can react with amine to form cova-
lent bonding of polymer-protein conjugation (Chinga-Carrasco &
Syverud, 2014). Poor suspension of nanocellulose in aqueous media
can be improved by grafting of acrylamide on nanocellulose sur-
face by redox inititation grafting method. The nanocellulose grafted
with acrylamide shows self assembly of lyotropic state (Yang & Ye,
2012). Hydroxyl groups of nanocellulose can be oxidized to dialde-
hyde by NaIO4 at appropriate experimental condition (Lu, Li, Chen,
& Yu, 2014). Surface of the nanocellulose can be modified by phos-
phorylation technique with phosphoric acid as negatively charged
phosphoryl donor (Kokol, Bozic, Vogrincic, & Mathew, 2015).
Dispersion and distribution of nanocellulose in the polymer
matrix can be improved by surface modification of nanocellulose
with appropriate molecules. In order to impart hydrophobic-
ity to the nanocellulose, a long hydrophobic alkyl chain can be
substituted from the hydroxyl functionality of nanocellulose via
bimolecular nucleophilic substitution (Bae & Kim, 2015). Benkad-
dour et al. proposed surface modification of oxidized nanocellulose
with long chain polycaprolactone diol (PCL) using click chemistry
and esterification reaction. Higher grafting yield can be observed
with click chemistry as compared with the esterification reaction.
PCL grafted nanocellulose with improved hydrophobicity could
be suitable for the reinforcement in the hydrophobic polymers
(Benkaddour, Jradi, Robert, & Daneault, 2013). Bacterial nanocellu-
ose can be modified with xyloglucan (XG) and xyloglucan bearing a
GRGDS pentapeptide to improve the wettability and cell adhesion.
Modified bacterial nanocellulose could be a potential candidate of
new biomaterial (Bodin et al., 2007).
5. Application of nanocellulosic materials
5.1. Biomedical applications
Scaffolds that could be prepared by using bacterial nanocellu-
lose (BNC) is ideal for many biomedical applications due to their
unique characteristics such as high porosity, excellent wet mechan-
ical properties, noncytotoxicty, and biocompatibility (Hong, Wei,
& Chen, 2015, Innala et al., 2014; Kramer et al., 2006; Krontiras,
Gatenholm, & Hagg, 2015, Kuzmenko, Samfors, Hagg, & Gatenholm,
2013; Sundberg, Gotherstrom, & Gatenholm, 2015; Nimeskern
 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316
et al., 2013; Park, Lee, & Hyun, 2015; Pretzel et al., 2013; Taokaew
et al., 2013; Moritz et al., 2014; Mueller, Wesarg et al., 2014;
Martinez Avila et al., 2015). 2,2,6,6-Tetramethylpiperidine-1-oxyl
(TEMPO) oxidized nanocellulose film exhibits excellent cell adhe-
sion and proliferation to be used as a potential candidate for
the development of biomaterials (Hua et al., 2014; Park et al.,
2015; Zander, Dong, Steele, & Grant, 2014). Further, TEMPO
oxidized bacterial nanocellulose can be used to prepare the hydro-
gel with elastin likes polypeptide (ELP). Positively charged ELP
would behave like a polymeric crosslinker with negatively charged
nanocellulose. Hybrid hydrogel has properties like noncytotoxic-
ity and capability to encapsulate cells that could find the potential
applications in the biomedical fields (Cheng, Park, & Hyun, 2014).
Chinga-Carrasco and Syverud reported pH sensitive nanocel-
lulose hydrogel which could be prepared from the surface
functionalized wood nanocellulose (Chinga-Carrasco & Syverud,
2014). Bacterial nanocellulose scaffold with excellent porous archi-
tecture has good mechanical properties, maintain a structural
integrity, excellent biocompatibility, supports cell in growth, and
secures tissue integration could be used for the auricular carti-
lage reconstruction (Avila et al., 2014; Martinez Avila et al., 2015;
Martinez Avila et al., 2014). Avila et al. reported bacterial nanocel-
lulose and alginate biphasic porous scaffold for the auricular
cartilage reconstruction (Avila et al., 2015). Bacterial biosynthe-
sized nanocellulosic hydrogel in static mode shows an extracellular,
highly crystalline cellulose molecules, and a flat shaped hydrogels
at the surface of the culture medium. The structure formed by irreg-
ular alignment of the BNC nanofibers is similar to those of collagen
matrices. However, small and heterogeneous pore size of scaffold
limits its use as implant material for the tissue engineering due
the difficulty in growth of cells. Laser patterning could make scaf-
fold favorable to support cell in growth for the cartilage remodeling
for the joint (Ahrem et al., 2014). Bacterial nanocellulose construct
has excellent properties such as tissue regeneration, faster heal-
ing properties, shape stability, controlled drug delivery etc. and all
these required for large skin transplantation, wound dressing and
reconstructive surgery (Fu et al., 2013; Moritz et al., 2014; Mueller,
Zink et al., 2014). The favorable biomedical property of bacterial
nanocellulose and the conductive property of polypyrrol could tai-
lored the nanocomposite for the tissue engineering which require
electrical conductivity such as nerve tissue reconstruction (Muller
et al., 2013).
Apart from the kidney transplantation, haemodialysis remains
other treatment method for the patients with chronic renal
failure. Polymer nanocomposite membrane could be prepared
with conductive polypyrrole and nanocellulose for haemodialy-
sis membranes. The nanocomposites membrane could combine
the active ion exchange and passive ultrafiltration with the large
surface area (Ferraz, Carlsson et al., 2012; Ferraz et al., 2013;
Ferraz & Mihranyan, 2014; Ferraz, Stromme et al., 2012). Fur-
ther, nanocellulose-polypyrrole composite membrane could be
an excellent candidate for the applications in electrochemically
controlled extraction and separation of biologically interesting
compounds (Nystrom et al., 2010). Razaq et al. proposed highly
porous polypyrrol-nanocellulose composite ion exchange mem-
brane for the solid phase extraction of biomolecules by reversible
electrochemically controlled process. Polypyrrol layer in the com-
posite membrane ensured excellent access to the ion exchange
molecules (Razaq, Nystrom, Stromme, Mihranyan, & Nyholm,
2011).
Microporous cellulosic hydrogel has the capability to function-
alized biomolecules and could find potential application for the
wound healing. Nanocellulosic hydrogel with smart pH respon-
sive property for biosensing can manage chronic wounds for
controlled and intelligent release of antibacterial components
(Chinga-Carrasco & Syverud, 2014). Ultrafine and extremely pure
307
fibrous network structure of silk sericin releasing bacterial nanocel-
lulose gel prepared at an appropriate culture media could find
applications in facial treatment. Silk sericin has many interesting
properties for biomedical applications such as biocompatibility,
antioxidant, bioadhesive, and bioactive activities. Further, the bio-
material shows excellent mechanical properties comparable to
that of the commercial paper mask, biodegradability, less adhesive
than paper mask (therefore, can be easily removable without pain)
and noncytotoxic (Aramwit & Bang, 2014). Nanocellulose based
modified superabsorbent polymer composite could be used as
biomedical application for drug delivery unit (Anirudhan & Rejeena,
2014; Lin, Bruzzese et al., 2012). Shape memory aerogel with an
excellent water absorption (due to the presence of numerous sur-
face polar group viz. hydroxyl and carboxylic groups) capacity
can be prepared by using the modified nanocellulose in a freeze
drying method. The aerogel retain excellent physical integrity in
water, while, demonstrating full and repetitive shape recovery
with repeated cycles required for biomedical applications (Jiang
& Hsieh, 2014). Nanocomposite prepared by modified nanocellu-
lose and collagen could be used for the tissue engineering scaffold
due its excellent biomedical properties such as biocompatibility,
cell adhesion and proliferation (Lu et al., 2014).
Other applications of nanocellulose in the biomedical field
includes, silver nanoparticle containing porous three dimensional
network structure of bacterial nanocellulose construct could find
the applications for the antimicrobial wound dressings. Silver
nano-particle can be immobilized by chemical linkage on porous
nanocellulose network which can prevent the release of nano
particles from the network structure (Berndt, Wesarg, Wiegand,
Kralisch, & Mueller, 2013). Antibacterial property of nanocellulose
could be improved by allicin and lysozyme. Allicin and lysozyme
conjugated nanocellulose possesses a good antifungal as well as
antibacterial effects, which could be useful to prepare antibac-
terial fabrics for the medical textile applications (Jafary, Mehrizi,
Hekmatimoghaddam, & Jebali, 2015; Jebali et al., 2013). Favorable
surface chemistry, morphology, rheology and ability to inhibit bac-
terial growth are useful characteristics of nanocellulose required
for the bio ink in 3D printing of porous wound dressing material for
potential to carry and release antimicrobial components (Rees et al.,
2015). Bio ink based on nanocellulose and aliginate for the potential
use of bio printing of biomaterials is proposed by Markstedt et al.
The developed bio ink is able to print both 2D and 3 D construct of
shaped cartilage structures (Fig. 5), such as a human ear and sheep
meniscus etc. (Markstedt et al., 2015). As a coordinated process,
bone regeneration is mainly regulated by multiple growth factors.
Nanocellulose (NC) based biphasic calcium phosphate with 0.5%
NC loaded scaffold shows that the growth factors were released
from NC in a sustainable manner for the required period. Biphasic
scaffold showed higher cell attachment and proliferation behavior
which could be beneficial for improved bone regeneration (Sukul,
Nguyen, Min, Lee, & Lee, 2015). Nanocellulosic hydrogel scaffold,
containing both osteoconductive and osteoinductive properties
which could enhance bone regeneration. Slower degradation rate of
the scaffold is due to the presence of nanofibrillar cellulose, and the
slower degradation rate favored the sustainable release of simvas-
tatin (an osteoinductive molecule) to enhance osteogenesis (Sukul,
Min, Lee, & Lee, 2015).
5.2. Energy, environmental and water related applications
Nanocellulose and conductive electro-active composite mate-
rial retain both constituent’s unique responsive properties viz.
nanocellulose as a matrix provide flexibility, whereas electroactive
material provide electrical properties. The developed composite
material has potential applications for the flexible electrodes, flex-
ible display, biocompatible energy scavenging, and so on (Shi,
308 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316

Fig. 5. (A) 3D printed small grids (7.2 × 7.2 mm2 ) with Ink8020 after cross-linking. (B) The shape of the grid deforms while squeezing, and (C) it is restored after squeezing.
(D) 3D printed human ear and (E and F) sheep meniscus with Ink8020. Side view (E) and top view (F) of meniscus (Markstedt et al., 2015) [Reproduced with permission,
Copyright © 2015, American Chemical Society].

Fig. 6. a) Digital photographs of a PPy, Nanocellulose, and Graphene oxide (PNG) paper electrode showing its flexibility during bending. (b) Stress–strain curve for a PNG
paper electrode. (c) Cyclic voltammograms for PNG paper electrodes recorded with two different bending angles, i.e. 0◦ and 180◦ , at a scan rate of 20 mV s−1 (Wang, Tammela
et al., 2015) [Reproduced with permission, Copyright © 2015, Royal Society of Chemistry].

Phillips, & Yang, 2013). Aerogel based on nanocellulose with the
high surface area and surface charge can be used for the layer-by-
layer assembly on conductive polymer, carbon nanotube, titanium
dioxide, zinc oxide, aluminum oxide to enhance the charge capac-
ity, flexibility and mechanical properties for the application in
energy storage and other electronic applications (Hamedi et al.,
2013; Korhonen, Hiekkataipale et al., 2011). Conducting compos-
ites based on polypyrrol and nanocellulose could be applicable in
environmentally friendly energy storage devices with commer-
cially viable mass loadings, capacitances, and energy densities
(Fig. 6) (Carlsson, Sjodin, Nyholm, & Stromme, 2013; Tammela et al.,
2015; Wang, Carlsson et al., 2015; Wang, Tammela, Stromme, &
Nyholm, 2015; Wang, Tammela, Zhang, Huo et al., 2014; Zhang
et al., 2013; Mihranyan et al., 2012). Nanocellulose can be used
to prepare the rechargeable power sources based on unitized sep-
arator/electrode assembly (SEA) construct. Paper batteries based
on electrode made with cellulose nanofibrils (CNF)/multiwalled
carbon nanotubes (MWNTs) demonstrated ultra thin (hence,
high-mass loading) electrodes far beyond those accessible with
conventional battery technologies. Ultrathin electrode in combi-
nation with readily deformable CNF separators allows fabrication
of user friendly paper batteries via origami folding techniques
(Cho et al., 2015). The cellulose nanofiber paper-derived separator
membrane is an electrolyte-phillic, nanoscale labyrinth structure
formed by closely packed CNFs. The cellulose nanofiber paper
separator prepared with appropriate experimental condition con-
tained highly interconnected nanoporous network channels with
good mechanical properties, excellent separator properties with
 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316
improved cell performance (Chun et al., 2012). The CNF separator
tightly secure the interlocked electrode–separator interface. The
unique physico-chemical structure of the SEAs drastically improves
the mass loading of electrode active materials, electron transport
pathways, electrolyte accessibility etc. (Choi et al., 2014). Further,
incorporation of silica (SiO2) nanoparticles allows loose packing of
CNFs as a result of more porous structure which allows better ionic
conduction due to the tailored combination of nanoporous struc-
ture and separator thickness, and all these properties contributed
to the excellent cell performance of the separator membrane (Kim
et al., 2013).
Kang et al. reported an all-solid-state flexible supercapaci-
tors of bacterial nanocellulose, carbon nanotubes and ionic liquid
based polymer gel electrolytes with high physical flexibility, desir-
able electrochemical properties, excellent cyclability and superior
mechanical properties (Kang et al., 2012). Mechanically strong and
highly conducting composite of nanocellulose and carbon nanotube
can be prepared from the aqueous dispersion in the form of semi-
transparent conductive films, aerogels and anisotropic microscale
fibers. Excellent colloidal stability of aqueous dispersion provided
simple and cost effective method for self assembly of advanced
hybrid nanocomposites for energy applications (Hamedi et al.,
2014; Henry et al., 2015).
Nanocellulose based paper possesses superior optical clarity as
compared with the regular paper substrate. Transparent and con-
ductive paper can be prepared by deposition of titanium oxide,
carbon nanotube, silver nano-rod, tin-doped indium oxide, boron
nitride, silica nanoparticles, quantum dot and molybdenum disul-
fide on nanocellulosic paper substrate. Transparent conductive
paper could find potential applications in wide range of optoelec-
tronics viz. displays, touch screens and interactive paper, organic
solar cell, lithium ion battery, energy storage devices and so on
(Hu et al., 2013; Li, Zhu et al., 2015; Liu, Sui, & Bhattacharyya,
2014; Uetani, Okada, & Oyama, 2015; Wang, Xu et al., 2015; Xue
et al., 2015). Composite based on nanocellulose and polypyrrole
is a promising material for electronic applications due to its large
surface area and capability to store charges. Polypyrrole nanocel-
lulosic composite paper based energy storage device has several
advantages such as high cell capacitances, superior rate capabilities,
excellent cycling performances, high performance, light weight and
low cost (Kizling et al., 2015; Nystrom et al., 2010; Razaq et al.,
2012; Wang, Tammela, Zhang, Stromme et al., 2014). Nanocompos-
ite paper based on nanocellulose with surface carboxylic groups
and carbon nanotube has good mechanical properties, flexibile,
excellent electrical conductivity, inexpensive and environmental
friendly, and could find potential for a wide range of flexible elec-
tronics (Koga et al., 2013).
Ecofriendly, flexible and electrically conductive nanocompos-
ite of nanocellulose and polyaniline can be prepared by in-situ
polymerization for the applications of flexible electronic, antistatic
coatings, and electrical conductors (Liu et al., 2014; Nguyen Dang
et al., 2013). Wang et al. proposed a novel method of carbon aero-
gel anode preparation for the lithium battery. Carbon aerogel with
large open pores and high surface area can be prepared by pyrolysis
of three dimensional bacterial nanocellulosic hydrogel construct.
Carbon aerogel shows very good electrochemical performance in
terms of both capacity retention and rate performance required for
the lithium ion batteries (Wang, Schutz, Salazar-Alvarez, & Titirici,
2014). Kobayashi et al. proposed a three dimensional aerogel pre-
pared by acid induced gelation and super critical drying of liquid
crystalline nanocellulose which is extracted from wood cellulosic
biomass. The aerogel with high porosity, large internal surface area,
good mechanical and heat insulation properties could be used as
thermal, acoustic, or electrical insulators (Kobayashi, Saito, & Isogai,
2014). Properties of nanocellulose such as degree of crystallinity
and water sorption capacity may have significant influence on
309
Fig. 7. Absorption capacities (Cm) of the silylated sponge (18.9 wt% Si), determined
for a collection of organic solvents (filled symbols) and oils (empty symbols). The
sample was deposited at the surface of the liquid for 5 s (Zhang et al., 2014) [Repro-
duced with permission, Copyright © 2014, American Chemical Society].
the dielectric properties of nanocellulosic composite materials for
electrical insulator applications (Le Bras et al., 2015). Kaoline and
nanocellulose composite could be promising for the cost effective,
flexible, low surface roughness and porosity substrate for printed
electronic applications (Penttila, Sievanen, Torvinen, Ojanpera, &
Ketoja, 2013; Torvinen, Sievanen, Hjelt, & Hellen, 2012).
Jiang et al. proposed a Nafion and bacterial nanocellulose com-
posite membrane for the proton exchange membrane fuel cell
(PEMFC) and direct methanol fuel cell (DMFC). Annealing of com-
posite membrane significantly decreases the water uptake, volume
swelling ratio and methanol permeability, due to the increased
dense structure, while, increases the Young’s modulus and selec-
tivity (Jiang, Zhang et al., 2015).
Nanocellulose based adsorbent has the potential to effec-
tively remove toxic components from the aqueous waste water
(Anirudhan & Shainy, 2015; Anirudhan, Deepa, & Binusreejayan,
2015; Arsad & Ngadi, 2014; Hokkanen, Repo, & Sillanpa, 2013;
Kardam, Raj, Srivastava, & Srivastava, 2014). Anirudhan et al.
reported a composite adsorbent based on poly(itaconicacid)-
poly(methacrylicacid)-grafted nanocellulose/nanobentonite for
the removal of Uranium from the aqueous solution. Adsorption
capacity of resultant adsorbents increases with increasing car-
boxylic group concentration on the surface of adsorbents. Further,
high surface area enhanced the adsorption capacity of adsorbents
(Anirudhan, Deepa et al., 2015). Suman et al. proposed a composite
adsorbent based on nanocellulose −silver nanoparticles embed-
ded pebbles for the cost effective and reusable system for effective
removal of contaminants such as dyes, heavy metals and microbes
from the aqueous media. In the composite adsorbent, silver nano-
embedded pebbles remove or kill microbes, whereas, nanocellulose
remove the dyes and heavy metal (Suman, Kardam, Gera, & Jain,
2015).
The photocatalytically active and stable hybrid materials of bac-
terial nanocellulos and TiO2 can be used for the purification of water
and polluted air (Wesarg et al., 2012). Zhang et al. reported an
ultra light, flexible, hydrophobic as well as oleophillic sponge based
on nanocellulose and methyltrimethoxysilane sols which could be
prepared by freeze drying. The spongy adsorbents can adsorb a
wide range of toxic organic solvents and oils with capacities up
to 100 times of its own weight, depending on the solvent and
oil properties (Fig. 7). Silylated nanocellulose sponges has excel-
lent flexibility, and shape stability in oil and solvent (Zhang, Sebe,
Rentsch, Zimmermann, & Tingaut, 2014). Carbon aerogel could be
310 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316
Fig. 8. SEM images of polystyrene latex beads and swine influenza virus (SIV) particles following filtration on Cladophora cellulose membrane: a) 500 nm beads; b) 100 nm
beads; c) 30 nm beads; and d) SIV particles (Metreveli et al., 2014) [Reproduced with permission, © 2014 Metreveli et al. Published by WILEY-VCH Verlag GmbH & Co. KGaA,
Weinheim].
prepared by controlled pyrolysis of nanocellulose hydrogel con-
struct. Aerogel exhibits excellent oil adsorption capacity due to its
micro porous network structure, high surface area, ultra light den-
sity with hydrophobic property (Meng et al., 2015). The surface
modified aerogel with the silanes could be useful for the separation
of oil from the aqueous solution of water and oil. Modified aero-
gel material has light weight and hydrophobic in nature, therefore,
float on water surface at the same time absorb oil in order to sepa-
rate oil from the aqueous solution. The adsorbents could adsorbed
oil few times on its own weight and adsorbed oil can be recov-
ered, hence, the adsorbents are reusable (Cervin, Aulin, Larsson, &
Wagberg, 2012). Incorporation of nanoparticles into the nanocellu-
lose substrate produce novel nanocomposite which could be used
as potential detector to detect trace contaminants in aqueous solu-
tion. For an example, bacterial nanocellulose and gold nanoparticle
composite based detectors have light weight, flexible, shape stable
in aqueous acidic and alkalinie solution (Wei et al., 2015; Wei et al.,
2014).
Hydrophilic characteristic of nanocellulose is useful for the
preparation of hydrogel adsorbent. However, enormous hydroxyl
groups on the adsorbent surface cause aggregation, hence, lim-
its its application as adsorbents, and this could be improved
by surface modification of adsobents with selective molecules
(Anirudhan & Shainy, 2015). Modified nanocellulose based adsor-
bents with high surface area and engineered surface functionalities
could be used to recover useful biomolecules such as beta-Casein,
trypsin, lysozyme, immunoglobulin, hemoglobin, from the aque-
ous solution (Anirudhan, Gopal et al., 2015; Anirudhan & Rejeena,
2012a; Anirudhan & Rejeena, 2012b; Anirudhan & Rejeena, 2013a;
Anirudhan & Rejeena, 2013b; Anirudhan, Rejeena, & Tharun, 2013).
Nanocellulose has plenty of surface functional groups such as
hydroxyl groups which could be functionalized with appropriate
molecules for the selective removal of toxic biomolecules such as
Fumonisin B1, aflatoxin B1, humic acid etc. from the aqueous solu-
tion (Jebali, Ardakani, Sedighi, & Hekmatimoghaddam, 2015; Jebali,
Ardakani, Shandadi, Zadeh, & Hekmatimoghaddam, 2015; Jebali,
Behzadi et al., 2015).
Highly porous, free standing, and light weight sponge like
nanocellulosic aerogel can be prepared by freeze drying of aque-
ous suspension of nanocellulose. The surface morphology such as
porosity and surface area of aerogel can be controlled by nanocel-
lulose quality and concentration in the suspension (Chen et al.,
2014). The TiO2 -coated nanocellulose aerogels with photocat-
alytic activity is very useful for the water purification applications
(Kettunen et al., 2011). Titanium dioxide coated nanocellulose
aerogel has oleophilic property, low density and high adsorption
capacity to adsorb organic contaminant from the wastewater sur-
face (Korhonen, Kettunen, Ras, & Ikkala, 2011). Filter paper can
be prepared by highly crystalline nanocellulose. The filter paper
with tailored pore size distribution could be particularly suitable
for the removal of virus (Metreveli et al., 2014). Various polystyrene
latex bead sizes of 500, 100, and 30 nm (representing the virus size)
(Fig. 8) are filtered out by the porous crystalline nanocellulosic filter
paper.
5.3. Polymer nanocellulose nanocomposite
Nanocellulose could be an excellent environmental friendly
nanofillers for the reinforcement in the polymer matrix in order
to prepare nanocomposite due to its nontoxicity, biodegradabil-
ity, low density, excellent mechanical properties and nanosize
dimension with higher surface area, hence, a huge interface
with the matrix polymers (Abraham et al., 2012; Abraham
et al., 2013; Aitomaki & Oksman, 2014; Ching, Rahman, Ching,
Sukiman, & Chuah, 2015; Costa, Druzian, Souza Machado, de
Souza, & Guimaraes, 2014; Juntaro, Pommet, Mantalaris, Shaffer, &
Bismarck, 2007; Li, Mascheroni, & Piergiovanni, 2015; Khan et al.,
2014; Khan et al., 2010; Kose et al., 2011; Kuzina et al., 2013;
Qua & Hornsby, 2011; Saxena et al., 2012; Zhou et al., 2012; Lani
et al., 2014; Lee, Aitomaki, Berglund, Oksman, & Bismarck, 2014;
Lee et al., 2009; Li et al., 2014; Li et al., 2013; Li, Renneckar, &
Barone, 2010, Pereda et al., 2011; Reddy & Rhim, 2014; Tome et al.,
2013; Voronova et al., 2012). One of the major challenges for the
 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316
reinforcement of natural fillers e.g. nanocellulose in the polymer
matrix is the incompatibility between polar (due to extensive sur-
face functional groups) nanocellulosic fillers and nonpolar polymer
matrix. Enormous hydroxyl groups on the cellulose nanocrystals
(CNCs) limit their dispesibility in the hydrophobic polymer matrix.
Gwon et al. modified the CNCs using toluene diisocyanate (TDI) to
overcome the poor of dispersibility in the poly(lactic) acid (PLA)
matrix. TDI-modified CNCs (mCNCs) shows good dispersion in
the PLA matrix with improved interfacial interaction between the
nanofillers and polymer matrix, when nanocomposites were pre-
pared by solvent casting (Gwon et al., 2016). Crystallinity of the
PLA-CNC nano-composites increases with increasing CNC content
in the nano-composites which were prepared by melt compound-
ing and melt fiber spinning followed by compression molding,
indicating that CNC can act as nucleating agent in crystallization
process. In addition, incorporation of CNC increases storage modu-
lus of the PLA film and influences the glass transition temperature
(Sullivan et al., 2015).
Hervy et al. proposed a green composite prepared by using
bacterial cellulose (BC) and nanofibrillated cellulose (NFC) as rein-
forcement in epoxy matrix to prepare environmental friendly
nanocomposites. The environmental impact of the nanocomposites
were evaluated using life cycle assessment (LCA). Nanocellulose-
reinforced epoxy composites with high nanocellulose loading is
desirable to produce nanocomposite materials with “greener cre-
dentials” (Hervy et al., 2015).
Juntaro et al. modified the sisal and hemp fiber by bacterial
nanocellulose to be used as filler for the preparation of green com-
posite based on cellulose acetate butyrate (CAB) and poly-l-lactic
acid (PLLA) as a matrix. Nanocellulose modified fiber shows better
adhesion in the polymer domain structure, hence, subsequently
improves the mechanical properties of composites (Juntaro et al.,
2007). Nanocellulose reinforced polymer composite could be use-
ful as ecofriendly materials for packaging, agriculture, membrane
as well as in hygienic devices. Nanocellulose can be used to modify
the natural fiber to improve the mechanical and interfacial proper-
ties by filling the stria and increasing the bonding with interfibrils
of natural fiber (Dai & Fan, 2013).
Reinforcement of nanocellulosic filler into the noncrosslinked
and crosslinked natural rubber significantly improves the mechan-
ical properties, and increases the degradation rate as compared
with the original natural rubber. As expected, noncrosslinked
natural rubber degrades at faster rate as compared with its
crosslinked counterpart. Three dimensional network structure
of the crosslinked rubber entraped the nanofillers, which sub-
sequently restrict the degradation of the composite materials
(Abraham et al., 2012). Aerogel prepared from soya protein is brit-
tle, and limits its potential applications. The mechanical properties
of soya protein aerogel could be improved by reinforcement of
nanocellulose. Nanocellulosic composite aerogel has high surface
area, low density and good mechanical properties, and all these
improved properties make composite aerogel an useful candidates
for potential applications in packaging, thermal and acoustic insu-
lation, transport media, etc (Arboleda et al., 2013). Shape memory
materials have the capability of fixing a temporary shape and
recover to the original shape by the applications of external stimuli.
Shape memory polymers have many advantages as compared with
other shape memory materials (viz. ceramic, metal alloy etc.), such
as low cost, light weight, storable large deformation etc. Some of
the polymers such as segmented polyurethane shows shape mem-
ory properties. However, segmented polyurethane has low stiffness
as compared with the shape memory ceramic and metal alloy.
The mechanical properties of shape memory polyurethane can be
improved by reinforcement of nanocellulose in the polyurethane
domain structure (Auad et al., 2008; Auad et al., 2012).
311
Due to its nontoxic in nature, packaging materials based on
nanocellulose composite have great potential to enhanced quality,
safety, and stability of packaged foods (Khan et al., 2014). Non-
toxic and biodegradable biopolymer such as starch and chitosan
could be used to elaborate edible films or coatings to enhance
shelf life of foods. Water vapor permeability is an important prop-
erty for the edible films to prevent the food spoilage. Water vapor
permeability and antibacterial properties of biopolymers film can
be tailored by nanocellulose reinforcement in the polymer matrix
(Dehnad, Emarn-Djomeh, Mirzaei, Jafari, & Dadashi, 2014; Dehnad,
Mirzaei, Emam-Djomeh, Jafari, & Dadashi, 2014). Nanocellulose
reinforcement in the polymer improve the mechanical proper-
ties, whereas, reduces the elongation and water barrier properties
required for water barrier films. The nanocomposite biopolymers
films are environmental friendly as compared to their synthetic
polymer counterpart (Azeredo et al., 2010). Highly ordered struc-
ture of cellulose nanocrystal improves the mechanical property
of film, and the presence of crystalline nanocellulose believe to
increase tortuosity in the film, further, enormous hydroxyl groups
on the cellulose nanocrystal bind the water molecules strongly by
hydrogen bonding as a combined result of slower diffusion process,
hence, reduces the water vapor permeability of the film required
for food packaging (Costa et al., 2014; Khan et al., 2010).
Nanocellulose can be efficiently reinforced into the polymer
matrix by in-situ polymerization for the preparation of nanocom-
posite. Mabrouk et al. reported cellulose nanocrystal polymer
composite prepared by miniemulsion polymerization of acrylic
monomers in the presence of cellulose nanocrystal and methacry-
loxypropyl trimethoxysilane (MPMS) which act as a coupling agent.
Silanol groups on the surface of polymer particles enhance the
adsorption of nanocellulose by hydrogen bonding. During the film
formation process (when water evaporates), the physical interac-
tion may converted into chemical linkage by condensation reaction
between surface silanol groups of the MPMS and hydroxyl groups of
nanocellulose, hence, effectively reinforced the nanocellulose into
the polymer matrix (Ben Mabrouk et al., 2014). Ultimate property
of the nanocomposite would depend on proper dispersion, distri-
bution nanocellulosic filler together with the, interfacial adhesion
and the interactions between matrix and nanofillers (Chirayil et al.,
2014). Mechanical property of nanocellulose polymer composite
increased with the increase of nanocellulose concentration up to
threshold limit then decrease thereafter (Cho & Park, 2011).
Interesting properties of polyurethane foams make them ideal
for the potential application in various fields. However, improved
properties are required for the specific applications. Polyurethane
foam morphology in terms of cellular morphology, open cell con-
tent, foam density, and mechanical properties such as compressive
and tensile properties, and impact properties can be tailored by
nanocellulose reinforcement in the domain structure (Faruk et al.,
2014).
5.4. Other applications
Barrier properties of paperboard and paper can be improved by
using nanocellulose reinforced alkyd resin. Smoothness and den-
sity of the rough and open structure of uncoated paper surface can
be improved by the use of very low loading of nanocellulose in
the resin solution. Further, water barrier properties of the coated
paper could be improved due to the sealing of surface and con-
sequently, creation of surface layer with low porosity. Moreover,
water molecules could be strongly attached with the nanocellulose
by hydrogen bonding with the abundant hydroxyl functionalities
on the nanocellulose surfaces, hence, reduces the water transmis-
sion through the nanocellulose containing film (Aulin & Strom,
2013).
312 S. Mondal / Carbohydrate Polymers 163 (2017) 301–316
pH is an important parameter to be measured and monitor
for the aqueous solution in the area of clinical diagnostics, water
quality assessment, food processing and bioprocess fields. Cost
effective biocompatible pH sensors can be prepared by aqueous
phase synthesis of nanocellulose and dye conjugate (Chauhan et al.,
2014). Farjana et al. reported flexible conductive sensor based on
nanocomposite which was prepared by using bacterial nanocellu-
lose and carbon nanotube (Farjana et al., 2013).
Polymer dispersion containing crystalline nanocellulose has the
potential for the security printing, and the optical authentication.
The printed on a dark paper by using crystalline nanocellulose con-
taining polymer dispersion shows darker than background with
polarizers, however, brighter if viewed under crossed polarizers
(Chindawong & Johannsmann, 2014). Freeze drying method of
nanocellulose and sodium montmorillonite produces foam like
and honeycomb like aerogel structure which possesses excellent
thermal, mechanical (can retain at high temperature) and energy
absorption capability, and the aerogel could find applications in the
packaging of goods (Donius et al., 2014).
Low cost hybrid films prepared by extrusion of nanocellu-
lose and ZnO suspension with excellent UV blocking property,
lightweight and flexible substrate, could find applications in the
UV blocking filed which required transparent substrate (Jiang, Song
et al., 2015). Hybrids aqueous media of nanofibrillated cellulose
and titania nanoparticles can be used for the transparent coatings
where high wear resistance and UV blocking activities are required
(Schutz et al., 2012). Composite paper prepared by using nanocellu-
lose and reduced graphene possesses high electrical conductivity,
excellent mechanical properties in wet and dry condition, and
could have potential application in humid environment as conduc-
tors, antistatic coatings, and electronic packaging (Luong Nguyen &
Seppala, 2015).
Flexible film prepared by using Zeolite and nanocellulose has
excellent capacity to remove the thiol, hence, the film with excel-
lent mechanical property could be applicable for the packaging of
fruits, foods, and vegetables which releases significant concentra-
tions of odors (Keshavarzi et al., 2015). Nanocellulose and graphene
foams having light weight, good combustion efficiency can be used
to improve the energy efficiency of the building (Wicklein et al.,
2015). Nanocellulose can be used to modify the synthetic textile
substrate to improve the dye ability of fiber due to the abundance
of hydroxyl groups on the nanocellulose surface and modified fiber
could have better binding to the dye molecules (Nourbakhsh, 2015).
Conductive carbon fiber can be prepared by pyrolysis of polyacry-
lonitrile (PAN) in an inert environment. The electrical conductivity
of the carbon fibers can be enhanced with increasing nanocellu-
lose concentration in PAN matrix because of the more ordered
graphite structure which enhances the movement of the ␲ elec-
trons (Park, Lee, & Kim, 2013). Nanocellulose can be used to prepare
novel sorbent for the solid phase micro extraction of biomolecules
(Ruiz-Palomero, Soriano, & Valcarcel, 2014, Ruiz-Palomero, Sori-
ano and Valcarcel 2015). ␤-cyclodextrin modified nanocellulose
(CD-NC) sorbent material prepared by using amidation reaction
of amine modified nanocellulose is highly efficient and selective
against danofloxacin (DAN) which is an antibiotic used to treat
animal diseases (Ruiz-Palomero et al., 2015).
6. Conclusions
In this paper, author reviewed the researches on the nanocel-
lulosic (NC) materials. Nanocellulosic materials have many
interesting properties (such as nontoxicity, biodegradability,
renewability, biocompatibility etc.) which make them ideal candi-
dates for many potential applications. NC can be extracted from the
lignocellulosic biomass by using various methods which influences
their properties. There are enormous potential for the nanocellu-
losic materials which includes nanocomposites membrane, hybrid
film, hydrogel, aerogel etc. are few of many to states. Cellulose
nanomaterials could have wide applications in food packaging,
energy, water treatment, biomedical filed etc. Further, nanocellu-
lose derived from the bacterial synthesis has proven as a promising
biomaterial for various biomedical applications such as tissue
engineering, drug delivery, wound dressing, cardiovascular appli-
cations etc. Author do hope that comprehensive literature review
on nanocelluloses presented in this paper will promote further
researches for the utilization of huge renewable lingocellulosic
biomass for the preparation of nanomaterials which could be useful
in diverse applications.
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