Journal of Saudi Chemical Society (2018) 22, 949–978

King Saud University

Journal of Saudi Chemical Society

www.ksu.edu.sa
www.sciencedirect.com

REVIEW

Materials chemistry and the futurist eco-friendly

applications of nanocellulose: Status and prospect
Raghvendra Kumar Mishra a,*, Arjun Sabu b, Santosh K. Tiwari c

a
International and Inter University Centre for Nanoscience and Nanotechnology, Mahatma Gandhi University, Kottayam,
Kerala, India
b
Centre for Biopolymer Science and Technology, Kochi, Kerala, India
c
Department of Applied Chemistry, Indian Institute of Technology (ISM), Dhanbad, Jharkhand, India

Received 29 December 2017; revised 12 February 2018; accepted 18 February 2018

Available online 23 February 2018

KEYWORDS Abstract Cellulose, a linear biopolymer, is present naturally in all plants. Apart from being the
Nanocellulose; planet’s predominant natural polymer, it also offers a variety of features including excellent bio-
Extraction; compatibility, lower density, substantial strength and the most beneficial mechanical characteristics,
Processing; inexpensive in cost. Applying the mechanical or chemical techniques, cellulosic materials are trans-
Composites; formed into cellulose nanofibres (CNFs) and even cellulose nanocrystals (CNCs). These CNFs and
Properties and application CNCs exhibit excellent capabilities in comparison with native cellulose fibre. Nowadays, nanocel-
lulose is being used in a variety of practical applications such as product packaging, papers as well
as paperboard, food sector, healthcare, hygiene products, paints, skin care products and sensors.
The current review article summarizes the cellulose, processing methods for nanocellulose, tech-
niques used for chemical modification of cellulose surface and consequently its application as rein-
forcement in polymeric materials. This article also provides a comprehensive discussion of the
historical development in the area of nanocellulose.
Ó 2018 King Saud University. Production and hosting by Elsevier B.V. This is an open access article under
the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 950
2. Cellulose. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 952
2.1. Hierarchical structure of cellulose. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 953

* Corresponding author.
E-mail address: raghvendramishra4489@gmail.com (R.K. Mishra).
Peer review under responsibility of King Saud University.

Production and hosting by Elsevier

https://doi.org/10.1016/j.jscs.2018.02.005
1319-6103 Ó 2018 King Saud University. Production and hosting by Elsevier B.V.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
950 R.K. Mishra et al.

3. Nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 955
3.1. Prehistory of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 955
3.2. Bacterial nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 957
3.3. Micro fibrillated cellulose (MFC) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 958
3.4. Nanofibrillated cellulose (NFC) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 958
3.5. Cellulose microcrystalline (MCC) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 959
3.6. Cellulose nanocrystals (CNCs) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 959
4. Nanocellulose preparation methods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 960
5. Nano cellulose fibers and interfacial problems . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 961
6. Surface modification of nanostructured cellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 962
7. Characterization of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 963
7.1. Microstructure of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 963
7.2. Thermal properties of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 965
7.3. Degree of polymerization of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 965
7.4. Irreversible agglomeration effect of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 965
7.5. Film formation properties of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 965
7.6. Surface area of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 965
7.7. Crystallinity of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 967
7.8. Oxygen barrier properties of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 967
7.9. Rheological characteristics of nanocellulose. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 967
7.10. Permeation properties of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 967
7.11. Toxicity effect of nanocellulose. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 967
7.12. Mechanical properties of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 967
7.13. Biodegradability of nanocellulose . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 968
8. Application of nanocellulose. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 968
8.1. Barrier for liquid and gaseous materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 968
8.2. Biomedical application . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 968
8.3. As reinforcement in polymer matrix . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 968
8.4. Nanocellulose for water purification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 968
9. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 970
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 970
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 970

1. Introduction and combination of hemicellulose and lignin as the matrix

The primary source of cellulose is natural fibres. In the early
phase of the nineteenth century, the chemical structure of cel-
lulose was identified followed by the in-depth research activi-
ties concerning cellulose. The chemical structure of cellulose
offers the advantage of being tailored such that new character-
istics can be achieved for several applications [1]. As shown in
Fig. 1, the evaluation shows that academic/research institutes
are performing the sheer range of activity on the cellulose as
well as nanocellulose in last 10 years.
In general, cellulose and other non-cellulosic constituents
serve as the building blocks for natural fibres. The cellulose,
which forms the principal constituent in natural fibres, can
be naturally extracted. The non-cellulosic constituents present
in natural fibres mainly include hemicellulose, lignin and pec-
tin. It is well known that wood is widely used for several appli-
cations because of its potential characteristics, which fulfil the
end-use performance [2]. The characteristics of wood are
dependent on several factors such as size, shape, composition
and configuration of cell walls. The nature of cell wall defines
the load bearing characteristics of wood fibres. It is important
to have favourable nature of cell wall in fibres as they hold its
reinforcement properties. It is primary to describe that the cell
wall composition of wood fibres itself acts as a composite con-
taining microfibrils of cellulose as the reinforcing component
component [3]. The cellulose microfibrils, which act as a rein-
forcing component, provide crystallinity and strength to the
cell. The microfibrils configuration in cell wall exists as a
mesh-like assembly. Each microfibril is connected to one
another via binding agent namely hemicellulose. Lignin, which
acts as the matrix phase is made of phenolic polymer and it
occupies the void space between cellulose, hemicellulose and
pectin compounds [4]. The cell wall is divided into the primary
and secondary cell wall. The pectin is present in middle
lamella, which acts as a binding agent for the interaction of
primary cell wall with that of adjacent plant cell walls. Fig. 2
shows the structure of cell wall.
In the recent times, cellulose gained substantial considera-
tion for the role of an innovative material in the area of green
chemistry for a number of end-use applications. Cellulose is
comprised of b-(1, 4)-d-glucose polymeric chains in a linear
manner. A number of units of b-(1,4)-d-glucose are gathered
to develop microfibrils of crystalline cellulose [5]. The biosyn-
thesis method leads to the development of crystalline microfib-
rils, which offer to strengthen effect to the cell wall. As the
result of extraordinary capabilities of nanocellulose (e .g. water
grasping as well as biocompatibility aspects), it is tremen-
dously recommended by the scientific circle, that is interested
in innovative green materials for numerous applications.
Hemicelluloses suggest a heterogeneous group of branched
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 951

Fig. 1 Statistical data from worldwide a) Cellulose interest by region (Top 15), b) Nanocellulose interest by region (Top 15) (From
google database- 2004 to present).

Fig. 2 Illustration of plant cell wall.

952
polysaccharides that are significantly less stable in comparison
with nanocellulose. nanocellulose is usually known as the
native cellulosic constituent with a unit size below one hundred
nm (in at least one dimension).Physical along with chemical
features associated with the material is believed to be essential
for its application in the range of areas [6].
Research has pointed out that cellulose-based materials
employed in the composite system provide excellent physical
as well as chemical features together with environmentally
friendly capabilities, which consequently turn them into ideal
materials for long-term practical application. Additionally,
the characteristics of nanocellulose based polymer nanocom-
posites have been discussed with regard to its possibility in
processing, performance as well as practical application. Poly-
mer nanocomposite is the term for the polymer matrix having
filler or reinforcement in at least one dimension in the nanome-
ter range (1 to 100 nm) [5]. Polymer nanocomposites manifest
incredible physical, chemically combined with thermal quali-
ties compared to traditional composites. Fundamentally, it is
nicely described that the attributes of nanocomposite are
decided by uniform distribution and dispersion of nanofillers
in polymer matrices as well as the interaction established
between them [7]. For that reason, many experts have stated
in a range of scientific studies that the dispersion, as well as
the distribution of nanofiller or reinforcement, is known to
be as crucial criteria to improve the characteristics of polymer
nanocomposites [8]. Because, the entanglements related to car-
bon nanotubes (CNTs) and consequently carbon nanofiber
leads to the self-agglomeration of these kinds of fillers in poly-
mer matrices, and consequently the functionality of polymer/-
carbon nanofibres and polymer/CNT composite systems is
interrupted. In an effort to prevent self-aggregation and to
enhance the proficiency of interaction among filler and the
matrix, modification strategies are employed to amend the sur-
face properties of nanomaterials. By means of surface treat-
ment method, it is also possible to establish hydrophilic or
hydrophobic features for the nanomaterials [9]. This is as a
result of covalent or even non-covalent interactions of fillers
with the polymer matrix, an improvement in properties of
nanocomposites are accomplished. In the recent years,
research activities are extensively carried out on the consump-
tion of various types of nanocellulose including (i) nanocrys-
talline cellulose obtained via acid hydrolysis and steam
explosion process and (ii) nano or microfibrillated cellulose
obtained via the mechanical process. These nanocellulose
materials have been utilized as reinforcement agent in polymer
matrices. The earlier studies experience difficulty in achieving a
homogeneous dispersion of nanocellulose in both water sol-
uble/insoluble polymer matrices [10]. In order to achieve a
homogeneous dispersion of nanocellulose in hydrophobic
polymers, chemical treatments are used to modify the surface
with the introduction of hydrophobic moieties. For example,
low molecular weight polymers or oligomers are adsorbed on
the surface of nanocellulose in order to achieve hydrophobic-
ity. The surface modification of nanocellulose presents several
advantages as it can enhance the interfacial adhesion among
nanocellulose and polymer matrix which in turn shows the
effect on the performance of nanocomposites [11].
From various kinds of nanocelluloses mentioned, extracted
nanocellulose materials are characterized by the sort of hydro-
gen bonding and microstructures of nanocellulose. These
microstructures vary with respect to processing routes and
R.K. Mishra et al.
sources of nanocellulose, for example, cellulose nanocrystals
(CNCs) obtained via acid hydrolysis process are represented
by bundles of rod-like crystallites [12]. Upon application of
supplementary processing or treatment methods, nanocrystals
can be formed. The micro-fibrillated cellulose (MFCs) exists as
interconnected nano-fibrillar structures. The exploitation of
several types of nanocellulose as reinforcements in the polymer
matrices has become intensely popular because it offers signif-
icant merits namely cheaper cost, biodegradability aspect, pos-
sibility to extract from sustainable resources, excellent
mechanical characteristics, barrier properties and a high
degree of surface polarity [13]. It has been noticed that the cel-
lulose and its derivatives are the safest materials used for appli-
cation in food as well as biomedical sectors [14]. In the case of
biomedical application, cellulose-based materials are used as
membranes for artificial kidneys and tissue engineering appli-
cations. With the aim to understand the role of nanocellulose
in various applications, the current review discusses types of
nanocellulose, tools used for characterizing the properties of
nanocellulose and addresses the challenges associated
with nanocellulose and its nanocomposites [15–17].
2. Cellulose
From the early period, cellulose possesses an exceptional posi-
tion in the catalogue of attracting materials that have been
used by the human beings. The ancient Egyptians employed
papyrus (an aquatic plant in form of a resource of cellulose)
to make writing materials/ paper, building carpets, ropes,
flip-flops, as well as containers. The very first time, French che-
mist Payen explained the chemical arrangement of the cellulose
in the early stages of the 19th century [18]. It was a milestone
research to investigate the study of cellulosic materials. In
recent years, plants serve as the most significant sources of cel-
lulose. Furthermore, cellulose can also be produced from
microbes and sea animals in larger quantities such as bacteria,
algae, fungi, tunicates and so forth [19]. Table 1 shows the dif-
ferent available sources for cellulose production.
From a definition point of view, cellulose is linear branch
polysaccharide (monosaccharides (sugar) monomer); it is pro-
duced from beta glucose monomers linked by 1–4 glycosidic
bonds with the degree of polymerization which ranges from
10 000 to 15 000 [25]. The bond produced between the two
monosaccharides that connected them is known as a glycosidic
bond. For example, all carbohydrates consist of carbon,
hydrogen and oxygen and also have the typical formula Cx(H2-
O)y [26]. Carbohydrates consist of compounds including sug-
ars, starch, glycogen and cellulose. Basic sugars have the
formula (CH2O)n, which means that the three component
are usually included in the identical ratio. Monosaccharides
are classified based on the value of n, that can vary from 3
to 7 for example Triose(n = 3), Tetrose(4 ), Pentose(5 ), Hex-
ose(6 ), Heptose(7 ) [27]. Glucose is the most typical hexose
and possesses the formula C6H12O6. Nevertheless, glucose
may have several distinct isomerisms. Glucose is able to
develop a straight molecule or a pair of distinct isomeric rings;
alpha glucose and beta glucose. These types of distinct struc-
tures possess completely different properties. Alpha glucose
molecules combine to develop starch, while beta glucose mole-
cules develop cellulose. The linear structure of the polymer
chain leads to the development of intrachain hydrogen bonds
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 953

Table 1 Main sources of cellulose.

Type of Remarks Ref.
source
Plants Plants remain as the significant source for cellulose production. This is mainly because of their abundance and cheaper [20]
nature. Plant-based resources include wood pulp, cotton fibres, bagasse, straw, ramie, sisal, flax, and hemp. Currently,
industrial facilities are available to harvest, process and extract cellulose from plant resources
Algae The most fundamental component present in cell wall of several algal species is cellulose. Green algae serve as the most [21,22]
suitable source for the extraction of cellulose. Also, red and yellow algal species are known to produce cellulose. It is
reported that the cellulose extracted from valonia and cladophoraspecies, which belong to Cladophorales and
Siphonocladales family, presents enormously high crystallinity of 95%. The characteristics of cellulose microfibrils are
dependent on the biosynthesis process that occurs in different algal species.
Bacteria The bacterial species namely Komagataeibacterxylinus is well known for the production of cellulose. This species [23]
utilizes carbon as well as nitrogen sources such that thick and clear cellulose microfibrils are formed on the growth
medium. The cellulose pellicles are further subjected to an alkali treatment to remove water followed by drying and
processing into membranes. The cellulose derived from microbes presents superior characteristics as compared to
cellulose derived from plant-based resources. These significances include (i) uniqueness in the nanostructure, (ii) a
greater degree of purity and (iii) higher mechanical properties.
Tunicates Tunicates belong to the family of marine invertebrates. They are capable of the production of cellulose in huge quantity. [24]
Enzyme complexes predominant in the epidermal layer of tunicates are responsible for the production of cellulose. The
characteristics of the produced cellulose are actually different with respect to species. The variation in the production
process of different species may affect the end characteristics of cellulose microfibrils.

between the hydroxyl groups together with oxygen atoms of

nearby ring molecules to balance the cellulose chains, and
the degree of polymerization is diversified relying upon the
source of origin [28].
Furthermore, the quantity, as well as characteristics of cel-
lulose, can vary with the characteristics of sources (e .g. wood
contained around 40 to 50% cellulose, and also cotton which is
90% cellulose) [29]. Tasteless, odourless, as well as
hydrophilicity with contact angle 20–300°, are the principal
characteristics of cellulose. The crystallinity together with Fig. 3 Schematic representation of cellulose.
amorphous transition temperature allows it to differ from
starch. Cellulose displays higher crystallinity compared to
starch, and also amorphous transition temperature is noticed
around 320 °C in water because of the crystalline character
of cellulose, another hand, starch possesses solely a transition
temperature above the 60–70 °C in water. Cellulose exhibits
kind of chirality and hydrogen bonds with water, however
because of the larger size; it is partially soluble in water and
insoluble in the majority of organic solvents. Additionally, glu-
cose units can be obtained from cellulose by the treatment of
the cellulose with concentrated acids at high temperature.
Fig. 3 shows the structure of cellulose [30].

2.1. Hierarchical structure of cellulose

It must be mentioned that the hierarchical structure of cellu-

lose is complicated. The primary fibrils are comprised of linear
cellulose chains and these types of fibril accumulate to generate
microfibrils and additionally combine to turn out as larger
macroscopic cellulose fibres [31]. These types of cellulose
fibres, lignin, and hemicelluloses put together to generate the
cell walls of wood as well as higher plants. All these cellulose
fibres interact as well as associated with lignin by the help of
hemicelluloses in form of a fibre reinforced composites system,
in which hemicelluloses behave as the binding agent for cellu-
lose fibre and lignin (matrix) [32]. A good number of
hydrogen-bond networks performs a vital role to arrange the
hierarchical structure of cellulose fibres, also hydrogen-bond
Fig. 4 Hierarchical structure of plant secondary cell wall.
networks are usually responsible for the improving the rigidity
of cellulose fibrils [33]. The cellulose is made up of two-phase;
these two kinds of phases are primarily two domains in the cel-
lulose chain referred as crystalline regions and amorphous
regions. Cellulose chains are organized in a significantly
ordered structure in the crystalline domain meanwhile amor-
phous regions indicate to the regions in which the chains are
randomly organized (high level of randomness as well as the
954
high degree of entropy) [34]. The hierarchical structure is
shown in Fig. 4.
On taking into account the groups of cellulose, the crys-
talline type of cellulose is principally classified in four distinct
polymorphs including (cellulose I, II, III and IV). Native cellu-
lose is specified by cellulose I and it is noticed that cellulose I
have two kind of polymorph which is dependent upon the
characteristics of the hydrogen bonding design; cellulose I a
(triclinic) or cellulose I b(triclinic) [35]. Cellulose Ia is obtained
from bacteria as well as algae, although, cellulose I b is
obtained from considerably higher plant sources. In addition
to, confirmation is used to explain the cellulose arrangement,
the trans and gauche conformation are the main kinds of con-
formation in cellulose configuration [21]. These types of con-
formations are seen in the group of rotary conformation, for
instance, tg, gg and gt, where t and g symbolize the trans
and gauche conformation, and arrangement of these particular
trans and gauche conformation is dependent upon the rotation
of hydroxymethyl group, which finally represents the structure
and character of cellulose [36].
There are several kinds of ways that have been employed to
transfer cellulose I into cellulose II etc. Mercerization is one of
them, currently employed to transform cellulose I into cellu-
(a)
Fig. 5 Scanning electron micrographs of the (a) wheat straw and (b) soy hulls fibres [40].
(a)
Fig. 6 Transmission electron micrographs of the (a) wheat straw and (b) soy hulls nanofibres [40].
R.K. Mishra et al.
lose II, the most stable type of cellulose by aqueous sodium
hydroxide treatment method or regeneration (solubilization
and recrystallization) [37]. Ammonia-treated cellulose I and
cellulose II is an additional processing method that could be
carried out to transform cellulose I and cellulose II into the cel-
lulose III and IV respectively. The various kinds of morphol-
ogy and crystalline structure of cellulose fibrils can be
achieved by using various chemical treatments, for example,
hydrolysis of cellulose by solid acid, alkali treatment, as well
as ammonia treatment [38].
The variation in crystallinity and allomorphism of cellulose
are characterized by employing the X-ray diffraction patterns
and solid-state 13C nuclear magnetic resonance (NMR) spectra
[39]. For instance, SEM images of wheat straw and soy hulls
are presented in Fig. 5a-b. Authors clearly stated that the
chemical treatment assists in the elimination of hemicelluloses,
lignin and pectin. Consequently, the average size of fibre bun-
dles without chemical treatment and with chemical treatment
was 25–125 lm and 10–15 lm respectively. The content of cel-
lulose extraction also differs with regards to the treatment
method and sources, the higher content of cellulose from
wheat straw fibres are obtained by acid and alkali treatment.
In order to, TEM morphology shows the microstructure of
(b)
(b)
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect
chemical–mechanical (cryo crushing, disintegration, and defib-
rillation) treated cellulose fibres of wheat straw and soy hull
fibres, as shown in Fig. 6. The figure suggests the separation
of the nanofibres from the micro-sized cellulose fibres.
Recently, it has been discussed that generation of nanoscale
cellulose from natural fibres is advantageous due to the nanos-
cale cellulose that provides much better performance than bulk
materials. The number of scientists’ attempts made it possible
to create various kinds of nanometric cellulose particularly
nanowhiskers, cellulose nanocrystals, NCC (nanocrystalline
cellulose), monocrystals, microcrystals or even the microcrys-
tallites and so forth [40].
3. Nanocellulose
The expression nanocellulose describes the cellulose fibril or
crystallite containing at least one dimension in the nanoscale
range, and it can be received by means of chemical or mechan-
ical treatment of the wood pulp or plant cellulose and so on
[41]. The use of nanocellulose is actually reliant on the struc-
tural –properties relationship. To render themselves for the
specific application of nanocellulose, they are widely catego-
rized in various sorts including cellulose microcrystalline
(MCC), micro-fibrillated cellulose (MFC), nano-fibrillated cel-
lulose (NFC), cellulose nanocrystals (CNC), nanorods or cel-
lulose whiskers and so on [5,42,43]. These types of
nanocellulose are obtained by changing their source like as
vegetable, lignocellulosic materials, bacterial cellulose, tunicate
cellulose, algae cellulose and so forth [44].
3.1. Prehistory of nanocellulose
‘‘Nano” is today’s scientific buzzword as well as TAPPI, in
the role of the world’s main cellulose technological company,
currently has founded a nanocellulose department [45]. The
world’s main cellulose technological company currently has
founded a Nanocellulose department. Therefore, what exactly
is nanocellulose, the way in which is it produced, what pre-
cisely can it accomplish, and what was the key reason, it
wasn’t it utilized before? Because the Chinese learned how
to create paper in a hundred and fifty B .C., cellulose experts
have noticed that cellulose in plants, as well as crops, consists
of millimetre-size fibres comprised of progressively more com-
pact microfibers and also microfibers which contain microfib-
rils of nanometer sizes and develop the fundamental building
blocks of cellulose from almost all sources . Scientists were
assured that nanosize microfibrils might have enormous sur-
face areas together with robust bonding, leading to brand
new products with greatly enhanced strength and also func-
tionality abilities [46]. As an example, making use of a gently
controlled pulp to create a good paper through including
small quantities of nanocellulose fibrils with their huge fibre
bonding ability.Unfortunately, nobody had actually created
any kind of nanocellulose from plants, nothing was available
for sale, and there were absolutely no books and guides acces-
sible to describe how to produce it. Therefore >2000 years,
nanocellulose was simply an idea for scientific theoretical dis-
cussion like a kind of ‘‘holy grail” for cellulose experts. In
reality, nobody had any specific concept of exactly what
nanocellulose from pulp should appear like even though they
discovered it [47].
955
In 1977 an investigation supervisor at the ITT Rayonier
Eastern Research Division (ERD) Lab in Whippany, N .J.
the USA, who employed a Gaulin-type milk Homogenizer to
create edible morning meal sausage casings from cowhides,
thought to operate a 3% slurry of chopped pulp fibres by
means of a high-pressure Manton Gaulin Milk Homogenizer
[48]. Due to the fact, the slurry attained 80 °C at 8000 psi;
the fibres have begun to experience a complete phase transfor-
mation and also converted into a translucent, firm ‘‘gel” which
they referred to as microfibrillated cellulose (MFC). In fact, at
the high temperature, the high forces (pressure/cavitation/she
ar/impact) of the homogenizer consequently had split up the
cell walls of the microfibers and also produced the preferred
nanofibrils. Certain scientific studies eventually started which
this rigid gel Rayonier was describing microfibrillated cellulose
was, in fact, the lengthy sort-after nanocellulose, which had
been separated by a basic technique with a small reduction
in (10%–15%) DP (degree of polymerization) [49]. The Ray-
onier investigation endeavours were introduced in a couple
of articles at the Ninth International Cellulose Conference at
Syracuse University (1981). In 1982–1983, worldwide eco-
nomics compelled ITT to shut down both Rayonier labs as
well as restrict additional work in this field, however, eleven
patents had granted involved in the production as well as
applications of MFC. Although Rayonier presented its pulp
clients free of charge license to these types of patents, there
might be a small question that the Rayonier MFC break-
through was the rise of a completely brand new sector of cel-
lulose technological innovation, i .e. nanotechnology. For the
subsequent thirty years, almost all nanotechnology beginning
gels and also advancements with regards to employing the
MFC high-pressure homogenizer technique at certain point
achieved positive results because of this discovery [50].
Acid hydrolysis of nanocellulose generates nanocrystalline
cellulose (NCC) rods which are suitable for producing items
with extraordinary characteristics as they are presently under
investigation. A lot of companies started to be active in the
area and the several patents and also a couple of articles pub-
lished by the Rayonier group in 1983 developed to 825 by 2007
which is greater in number nowadays. A variety of companies/
institutions used derivatized, hydrolyzed, pre-swollen, enzyme-
treated, oxidized and also tailored pulps in the role of feed-
stocks with purpose designed 30,000–45,000 psi homogenizers
to lesser energy demands and also wide nanoparticle-size dis-
tributions, that has mutually changed MFC into NFC [51].
It is possible to form nanocellulose by subjecting the microfib-
rils to physical or chemical treatments such that crystalline
regime of cellulose could be extracted. The nanocelluloses are
composed of crystalline cellulose units in rod-like form. The
other nomenclature for nanocelluloses includes nanowhiskers
and microcrystallites. The nanocelluloses exhibit high surface
area and mechanical properties.Cellulose particles exist in
two forms namely (i) Nanocelluloses and (ii) Micro-
fibrillated cellulose (MFC) [90]. The different types of termi-
nologies used for describing nanocelluloses, their origin and
processes used for the production of nanocelluloses are pre-
sented in Table 2.
In general, nanocellulose is obtained from renewable poly-
mers via acid hydrolysis. The nanocelluloses have gained the
attraction of scientific community due to their significant char-
acteristics like rod shape, tunable surface chemistry, high
mechanical strength and sustainable nature. In the recent
956 R.K. Mishra et al.

Table 2 Different types of terminologies used for describing nanocelluloses, their origin and processes used for the production of
nanocelluloses.
Type of cellulose Origin Extraction process Ref.
Cellulose Crystallites Whatman filter paper HydrolysisusingH2SO4 [52]
Microcrystalline cellulose Alpha-cellulose fibres Hydrolysis [1]
Microfibrillated cellulose Pulp Gaulin Homogenizer [53]
Cellulose nanocrystals Whatman filter paper, cotton woodland Hydrolysis usingH2SO4 [54]
bacterial cellulose
Cellulose Nanocrystals Microcrystalline cellulose Sonication or H2SO4 hydrolysis [55]
Whiskers(rod-like nanoparticles) Cellulose fibres H2SO4 hydrolysis [55]
Cellulose nanowhiskers Ramie, microcrystalline cellulose H2SO4 hydrolysis [56]
Cellulose nanowhiskers Cotton Hydrolysis using HCl [57]
Nanocrystalline cellulose Microcrystalline cellulose Hydrolysis using H2SO4 [58]
Nanocellulose Sisal fibres H2SO4 hydrolysis [59]
Nanofibrillated cellulose, Cellulose Sulfite pulp Mechanical route [60]
nanofibrils
Microcrystalline cellulose Alpha-cellulose fibres Hydrolysis [61]
Cellulose Microcrystal Whatman filter paper Hydrolysis using HCl [62]
Microfibrillated Cellulose Sulfite pulp Mechanical [63]
Nanofibres Soybean Chemical treatment and defibrillation under [64]
high pressure

Table 3 Dimension of various types of nanocellulose.

Cellulose structure Diameter (nm) Length (nm) Aspect ratio (L/d) Ref.
Microfibril 2–10 >10,000 >1000 [68]
Microfibrillated cellulose (MFC) 10–40 >1000 100–150 [67]
Cellulose whisker 2–20 100–600 10–100 [69]
Microcrystalline cellulose (MCC) >1,000 >1000 1 [70]

Table 4 Types of nanocellulose.

Type of Designation Sources Average size Ref.
nanocellulose
Cellulose Nanocrystalline cellulose Wood, cotton, hemp, flax, wheat straw, rice Diameter: 5–70 nm [1]
nanocrystal (NCC), whiskers, rod-like straw, mulberry bark, ramie, MCC, Avicel, Length: 100–250 nm (from plant); 100
(CNC) cellulose, microcrystals tunicin, algae, bacteria, etc. nm–several micrometres (from cellulose
of tunicates, algae, bacteria)
Micro/ Nanofibrils, microfibrils, Wood, sugar beet, potato tuber, hemp, flax, Diameter: 5–60 nm [71]
Nanofibrillated nanofibrillated cellulose, etc. Length: several micrometres
cellulose (NFC) Microfibrillated cellulose

years, nanocelluloses have been extensively used in several
biomedical purposes such as drug delivery, scaffolds for tissue
engineering, and biosensors [65]. Although several studies have
indicated that nanocellulose present the potential to be used in
biomedical applications, it is further required to investigate
the complete therapeutic potential of nanocelluloses in
real time [105]. Much attention has been drawn to investigate
the interaction of nanocelluloses in biological models
through in vitro and in vivo studies. Recently, the biocompati-
ble nature of cellulose derived from bacteria has been studied.
This study further clarifies the biocompatibility nature of cellu-
lose implants. The significant property of bacterial cellulose is
its physical structure, which can be readily controlled at differ-
ent scales (macro/micro/nano) in order to make it suitable for
biomedical purposes. In addition, efforts are underway to tune
the surface properties, porosity range and orientation of cellu-
lose fibres [82,89,106]. Apart from bacterial sources, plant-
based resources are also extensively investigated for the pro-
duction of cellulose nanocellulose. Plants serve as cheap
sources for the production of nanocellulose in large scale [66].
A summary of the dimension of nanocellulose materials is
outlined in Tables 3 and 4. Outstanding mechanical strength,
crystallinity, good possibility for chemical modification, bio-
compatibility, high specific surface area, biodegradability, high
aspect ratio, beneficial rheological, lightweight, exceptional
oxygen permeation and water- vapour transmission resistance,
oil grease barrier, aqueous liquid barrier, optical characteris-
tics and inexpensive in cost are the primary attributes of
nanocellulose [6]. These types of characteristics render
nanocellulose perfect for an array of applications in numerous
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 957

areas such as tissue engineering, electronic devices, food pack-

Table 5 The key application of nanocellulose in various fields.
aging, and medical devices (drug release and antimicrobial
Area of Key application Ref. packaging), as mentioned in Table 5 [67].
Application
Electronic Sensor, electronic displays and [72]
Devices windows
3.2. Bacterial nanocellulose
Construction Sensors to monitor stress levels in [73]
bridge Nanocellulose is a word dealing with nanostructured cellulose.
Food packaging Packaging for oxygen barrier [74] This can be cellulose nanofibres (CNF) known as microfibril-
Food products Stabilizer for suspension and flavour [75,76] lated cellulose (MFC), nanocrystalline cellulose (NCC or
carriers CNC), or bacterial nanocellulose, which is the term for
Paper products Grease-proof paper [77]
nano-structured cellulose created by bacteria. CNCs and
Composites Improve the mechanical properties [78]
of polymer matrix
CNFs are produced from natural sources (bacteria, tunicate,
Oil recovery Fracturing fluid in oil recovery [79] and wood) via common hydrolysis situations (acid, enzymatic,
Medical and Water absorbent pads, antimicrobial [80–82] mechanical, and TEMPO-mediated oxidation) [85]. CNCs
Tissue films and tampons, sanitary napkins which are rodlike in character possess a greater crystalline por-
engineering or wound dressing tion in comparison with CNFs that are fibrillar in character.
Cosmetic Composite coating agent for nails, [83] Sizes and aspect ratios of the CNCs evaluated are based on
hair, eyebrows or eyelashes the source of the cellulose. In the scenario of bacterial-
Automobile Lightweight and high [84] sulfate, the longer fibres were additionally thicker, maintaining
strength components such as their aspect ratio low [85]. The relationship between these types
bumpers, side panels and dashboards
of nanocellulose is shown in Fig. 7.

Fig. 7 Relationship between different kinds of nanocelluloses [85,86].

958
Bacterial nanocellulose (BNC) is a rising nanomaterial with
extraordinary properties derived from various species of com-
mon fermentation bacteria, particularly Gluconacetobacter
xylinus . BNC has been employed for a number of industrial
applications such as textiles, cosmetics, and also food items,
and it possesses an excellent capability for healthcare applica-
tions [87]. BNC can be custom-designed with a remarkable a
number of patterns for example fleeces, foils, spheres, tubes,
fibrous aggregates or in form of produced pulp. Moreover,
remarkably crystalline needle-shaped nanocrystals are
achieved by acidic, oxidative or enzymatic degradation of the
amorphous fractions [88]. The extraordinary 3D nanofibrillar
network offers additional material properties dissimilar from
plant cellulose, for example, a prominently high mechanical
(Young’s modulus of single fibers: 2 GPa) and thermal
(around 300 °C) stability, higher moisture content (>90%),
crystallinity (70–90%) and degree of polymerization (up to
10 ,000 anhydroglucose units), along with an impressive
formability and softness [89] . There is an immense perspective
of bacterial nanocellulose in health care as well as drug appli-
cations, however recently the development of the innovative
functions, as well as advanced drug profiles, has quite retarded
[66]. Likewise, drugs with inadequate water solubility and/or
dissolution rate along with hydrolytically medicines involve
more complex development techniques in BNC, nevertheless
provide a vast area for applications which has still to be stud-
ied. The study is principally concentrated on material science
instead of on biological as well as medical proof-of-concept
tests, although it would need to be taken from the structure
and prototype phase to additional application-oriented tests
[90]. But, outcomes from a fundamental study on the percep-
tion of BNC in the role of drug carrier system may possibly
properly enhance the theme of BNC-mediated tissue regenera-
tion, medicine delivery systems, vascular grafts, and scaffolds
for tissue manufacturing in vitro and in vivo [91]. The benefits
of BNC are the higher cellulose purity in comparison to plant
sources, greater flexibility, better hydrophilicity, and also med-
icine load-release characteristics. The drawbacks are the pro-
longed production time, the necessity of axenic situations for
cultivating particular bacteria, and the reaction situations of
the biosynthesis [92,93]. Commonly, plant-derived nanocellu-
lose is derived from the top-down mechanical and/or chemical
procedure of cellulosic precursors. Conversely, bacterial
nanocellulose is derived from the direct action of particular
bacterial strains which belongs to genus for example Achro-
Fig. 8 Scheme for microfibrillated cellulose.
R.K. Mishra et al.
mobacter, Alcaligenes as well as Gluconacetobacter among
which simply Gluconacetobacter xylinus has been presented
to generate BC at industrial production levels [94]. Electrospin-
ning, as well as regeneration of cellulose acetate, are alternative
strategies to have nanocellulose [95].
3.3. Micro fibrillated cellulose (MFC)
Microfibrils cellulose is identified in form of fine cellulose hav-
ing multiple elementary fibrils, including the aggregated
crystalline-amorphous region with high aspect ratio as well
as surface area [96]. The disintegration of cellulose fibres into
micro range fibrils is referred to as cellulose microfibrils, con-
taining the dimension ranging from few microns, as shown
Fig. 8. Nevertheless, if fibrils possess a dimension ranging from
10 to 100 nm, it is assigned as nanofibrillated cellulose [97].
The mechanical properties are tailored via altering the
microstructure of micro or nanocellulose, as shown in Table 6.
3.4. Nanofibrillated cellulose (NFC)
Nanofibrillated cellulose (NFC) expression is employed to
express fibrils with dimension in the range of nanometric scale
that is primarily obtained from wood by means of mechano-
chemical treatment of wood pulp. NFC comprises of both
individuals as well as aggregated nanofibrils [104]. The primary
fibril is identified as 3–5 nm in diameter and around 500–1000
nm long, although the aggregated NFC is in the range of 20–
50 nm in diameter. Both amorphous and crystalline regions are
equally noticed in the NFC. The fundamental dissimilarity
between microfibrils and nanofibrils is the fact that, nano fib-
rillated possess finer diameter in comparison with micro-
fibrillated cellulose [105], as shown in Fig. 9. In 1983, Turbak
and Herrick extracted NFC from wood pulp. They employed a
high shear mechanical homogenization strategy; however, the
high-energy consumption was a serious problem for extracting
the NFC in the late 1980 s.Succeeding improvements led to
numerous techniques of pre-treating the cellulosic fibres that
have cut down the energy consumption up to 98%. The pre-
treatment is separated into two categories: (i) mild acid or
enzymatic hydrolysis and (ii) introduction of electrostatic
repulsion between the fibres, the electrostatic repulsion
continues to be accomplished by chemical modification of
the fibrils to generate anionic surface charges, e .g. car-
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 959

Table 6 Mechanical properties of nanocellulose [98].

Type of nanocellulose Yong Modulus (GPa) Characterization method Ref.
Nanofibril cellulose 81 ± 12 Atomic force microscopy tips(Mode of testing: Three points bending) [99]
Nanofibril cellulose 100 Tensile testing [100]
Bacterial Cellulose 114 The Raman spectroscopy (By analysing the local molecular deformation via [101]
a shift in the central position)
Nanocrystalline cellulose 139.5 ± 3.5 Nono indentation [102]
Nanocrystalline cellulose 206 Atomic structure model with the help of quantum mechanics [103]

Fig. 9 Various types of nanocellulose, a) Cellulose fibre, b) Fig. 10 Scanning electron microscopy morphology of micro-
Microfirbrillated cellulose, c) Nanocrystalline cellulose, d) Cellu- crystalline cellulose [109].
lose nanofibrils.

boxymethylation or 2,2, 6,6-tetramethylpiperidine-1-oxyl

(TEMPO)-mediated oxidation etc . The rheology of cellulose
nanofibrils gels is actually one of the key characteristics, which
permit cellulose nanofibrils to be applied in the food industry
and stabilizing dispersions [106]. Alongside, the cellulose
nanofibrils gel is produced by adding the low concentration
of cellulose nanofibrils in water. By separating the gel suspen-
sions and also making use of the dispersion casting strategies,
cellulose nanofibrils gel is transformed into thin films of cellu-
lose nanofibrils. Properties including high tensile strength, low
thermal expansion as well as the formation of an oxygen bar-
rier permit cellulose nanofibrils films in food and pharmaceu-
tical packaging, electronic devices, and printing applications
[107].
3.5. Cellulose microcrystalline (MCC)
Microcrystalline cellulose is identified as a high crystalline
structure of cellulose-containing aggregates of strongly
hydrogen-bonded bundles of multi-sized cellulose microfibril.
Considering the features of micro cellulose, microcrystalline
cellulose is the fine powder with particle sizes ranging between
10 and 50 mm in diameter. The primary source of cellulose
microcrystalline is craft wood fibres. Microcrystalline cellulose
is obtained from these types of sources with the aid of bleach-
ing and subsequent sulfuric acid treatment method [108]. The
morphology of the microcrystalline cellulose has been
reported, as shown in Fig. 10.
3.6. Cellulose nanocrystals (CNCs)
The term cellulose nanocrystal describes the rod-like nano-
crystal configuration. Acid hydrolysis method is used to erad-
icate the amorphous regions in the native cellulose, and the
remarkably crystalline region in native cellulose is commonly
unaltered by acid treatment method producing a rod-like
structure as cellulose nanocrystal (CNC) is achieved ultimately
referred to as nanocrystalline cellulose or cellulose whiskers [1],
as demonstrated in Fig. 11.
Cellulose nanocrystal bears the wide range of properties
including huge surface area, excellent stability, fascinating
mechanical (higher specific strength as well as modulus), and
also extraordinary optical properties. Cellulose nanocrystal
exhibits the comparatively high level of crystallinity around
(54–88%). The dimension of cellulose nanocrystal is dependent
upon the nature of the source, and normally, it possesses typ-
ical dimension 3–30 nm in diameter as well as 100 nm to 1–2
lm in length. It reveals that all dimensions of nanocrystalline
cellulose are actually in the nanometer size range. Nanocrys-
talline cellulose has been utilized in the role of mechanical
strengthening agents, medicine delivery vehicles, templates in
the synthesis of nanocomposite material as well as protein
immobilization substrate. Table 7 demonstrates the dimen-
sions of cellulose nanocrystals with regards to the source and
technique of extraction.
960 R.K. Mishra et al.

Fig. 11 Extraction of cellulose nanocrystal (CNC).

Table 7 Dimension of nanocellulose crystal with respect to the various parameters.

Method Source Remarks Ref.
H2SO4 hydrolysis Bacteria L(nm) = 100–1,000, W(nm) = 10–50, Aspect ratio (L/D) = 2–100 [110]
H2SO4 hydrolysis Valonia L(nm) = 1,000–2,000, W(nm) = 10–20, Aspect ratio (L/D) = 50–200 [111]
H2SO4 hydrolysis Ramie L(nm) = 70–200, W(nm) = 5–15, Aspect ratio (L/D) = 12 [112]
H2SO4 hydrolysis Wood L(nm) = 100–300, W(nm) = 3–5, Aspect ratio (L/D) = 20–100 [113]
H2SO4 hydrolysis Sisal L(nm) = 100–300, W(nm) = 3–5, Aspect ratio (L/D) = 60 [59]
H2SO4 hydrolysis Tunicates L(nm) = >1000, W(nm) = 10–20, Aspect ratio (L/D) = 100 [114]
HCl hydrolysis Bacteria L(nm) = 160–420, W(nm) = 15–25, Aspect ratio (L/D) = 7–23 [115]
HCl hydrolysis Cotton L(nm) = 100–300, W(nm) = 3–5, Aspect ratio (L/D) = 20–100 [116]

4. Nanocellulose preparation methods
Nanocellulosic fibres are derived from cellulose fibres by
means of a variety of treatment methods (e.g. chemical treat-
ment, mechanical treatment, as well as chemo-mechanical
treatment) of cellulose fibres. These types of treatments adhere
to some fundamental protocols: 1) pretreatment method of
cellulose source to gain cellulose fibres, as shown in Fig. 12.
The pretreatment procedure is used to taking out hemicellu-
loses as well as lignin, enhance the quality of cellulose, and
Fig. 12 Step 1 (Pretreatment of cellulose-containing materials)
for preparation of nanocellulose materials.
consequently improve the fibrillization as well as the transfor-
mation of the cellulose fibre into micro/ nanofibrils. Within
this sequence, mechanical treatment is an expensive process,
considering the fact that high-energy consumption is required
[117]. As a result, chemical treatment is primarily used to mini-
mize the energy consumption; a brief explanation of chemical
pretreatment process is stated just as streams. First, we men-
tioned the pretreatment process called as step first, as shown
in Fig. 12.The purpose of the pretreatment process is to take
out ashes, waxes, lignin, hemicellulose, as well as other noncel-
lulosic compounds that are important to generate pure cellu-
losic products such as cellulose nanofibrils and cellulose
nanocrystals. A pretreatment additionally decreases the energy
requirement of mechanical processes from 20, 000 to 30, 000
kWh/ton to 1000 kWh/ton. The kinds of pretreatments
employed on various raw materials for example tunicate,
algae, and bacteria cellulose have been discussed in the past.
The alkaline delignifications, as well as organosolvation with
acetic acid, aqueous methanol, or ethanol, are likewise viewed
as pretreatment techniques [118], as shown in Table 8.
After the step 1 (pretreatment); step 2 is needed for achiev-
ing the nanocellulose from pretreated cellulose fibres. Further-
more, different types of strategies are entirely applied to carry
out step 2, the mechanical, chemical and mechanical-chemical
route such as high-pressure homogenization, microfluidiza-
tion, micro grinding, high-intensity ultrasonication, electro-
spinning, and steam explosion are extensively employed
methods for carrying out step 2. The pros and cons of the var-
ious methods are pointed out in Table 9.
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 961

Table 8 An overview of the pretreatment process.

Method of Pretreatment Remarks Ref.
Alkaline Hydrolysis More efficient lignin, hemicellulose, and also pectin solubilization as well as extraction, lignin as well [119]
as hemicellulose are hydrolyzed, in case that lignin content is rich in the cellulosic source. Generally,
oxidation agents are employed to improve the efficiency of alkaline pretreatments process.
Acid Hydrolysis Break the rigid structure of the lignocellulosic component, comprises of includes concentrated as well [120]
as dilute acid solutions, this process is toxic, hazardous, and corrosive in nature, different types of
acid, pH, reaction temperature and reaction time has an influence on the final cellulose yield.
Organosolv Simultaneous degradation of lignin and hemicelluloses, not economically feasible, consumption of [121]
organic solvents
Ionic liquid Ionic liquid collapses intramolecular hydrogen bonds, high dissolution capacity, low/no toxicity, [122]
reduce crystallinity of cellulose
Oxidation(TEMPO-mediated Chemical pretreatment carried out under aqueous as well as the mild environment, helps prevent the [123]
surface oxidation) post aggregation of nanoparticles throughout the drying stage, takes away the separation of the
nanofibrils from one another because of the repulsive forces of the ionized carboxylate groups.
Enzyme Degrade the lignin and hemicelluloses contents, various type of enzymes are used such as [124]
cellobiohydrolases (A and B type, which attached on crystalline part of cellulose). Endoglucanases
(C and D types, which attack amorphous part)

Table 9 Significance and drawback of various processes.

Process Remarks Ref.
High-pressure It is generally free from organic solvent as well as effective method, nevertheless, blocking concern is the major [125]
homogenization problem, and it is defibrillation method based on the pressure.
Microfluidization It is equivalent as high-pressure homogenization, it is easy to use, this method does not significantly alter the [126]
kappa number of cellulose nanofibrils in comparison to original pulps, and nevertheless, it is not necessarily
appropriate at the industrial level.
Microgrinding Within this approach, shear forces are employed on split up of hydrogen bond as well as cell wall structure, it is [127]
a faster method and refining pre-treatment is crucial in this specific method. Nevertheless, this method changes
the crystallinity of cellulose nanofibrils.
High-intensity It is usually utilized to the obtaining a high rate of defibrillation, it is an effective method, there is the particular [128]
ultrasonication restriction, for example, this procedure is beneficial at laboratory scale, and also generate the high degree of
noise, and pretreatments are provided to discharge cellulose nanofibrils.
Cryocrushing A mechanical method for fibrillation of cellulose, this mentioned are performed with the help of liquid nitrogen [129]
and subsequently crushing.
Steam explosion Thermomechanical process(heat carried by steam), high-pressure steam penetrate the penetrates the [130]
lignocellulosic, shear force is generated by the sudden release of pressure which helps hydrolyze the glycosidic
bond and hydrogen bonds and produce nanofibres of cellulose.

5. Nano cellulose fibers and interfacial problems
The possible use of nanofibres is dependent upon its strength-
ening along with filler capability in the polymer matrix. The
inadequate dispersion limits its reinforcement capability in
the polymer matrix. One other issue generally observed is the
fact that agglomeration of the filler, particularly whenever it
is employed in form of nanofiller in thermoplastic polymers
[131]. The nano-dimensional with the huge specific surface area
and large value of thermodynamic potential (G) of the nano-
materials lead to the lack of stability of nano-sized materials.
According to thermodynamics, DG = r DS (where r is the
specific surface energy), it is well recognized that stability of
the system is described in the performance of its specific sur-
face area. Consequently, the excessive specific area of the
nano-sized materials allows for the development of bigger
structures by means of aggregation as well as the agglomera-
tion of nanomaterials [132]. As a result, the mechanical
features of the composites are negatively influenced by the
inadequate dispersion as well as distribution (aggregation
and agglomeration) of the filler in the polymeric matrices.
The active groups (–OH) exhibit on the surface of cellulosic
nanofibres possibly created the bonds with neighbouring –
OH group through weak hydrogen bonding [133]. This process
is related to the agglomeration or entanglement of the
nanofibres, this kind of entanglements can be found right here
Fig. 13. To prevent this issue, it is suggested to maintain the
nanofibres in form of the water suspension (polar suspension)
whenever it is received after chemo-mechanical treatments.
Due to the fact that cellulose nanofibres (CNF) possess robust
inclination to develop hydrogen bonds with adjacent fibrilla-
tion; it may possibly contribute to inadequate dispersion in
nonpolar solvents. An additional crucial issue related to
nanofibres is the concern of redispersion of nanofibres after
drying. It may extend to an irreversible aggregation of the fib-
rils that is related to the event referred as ‘‘hornification”, and
material displays ivory-like characteristics that are not advised
to employ for rheological purposes or in composite applica-
tions [134]. The fundamental strategy to prevent hornification
is the inclusion of a steric barrier or electrostatic groups to
962
Fig. 13 Cellulosic nanofibres extracted from coir fibre [135].
confine the combination of hydrogen bonds with neighbouring
fibrils of the cellulose chains. The lots of hydroxyl groups exist-
ing on the surface of cellulose nanofibres makes it possible for
the feasible efforts to the addition of various chemical
modifications, as well as esterification, etherification, oxida-
tion, silylation, polymer grafting, and so forth [39].
The chemical functionalization techniques primarily high-
lighted the addition of stable negative or even positive electro-
static charges on the surface of cellulosic nanofibres, which
assists to achieve beneficial dispersion as well as the strength-
ening of nanocellulose in polymer matrices [136]. Furthermore,
the chemical functionalization tunes the surface energy of cel-
lulosic nanofibres and therefore enhances the compatibility,
particularly in thermoplastic polymers. It is usually noticed
that the surface alternation can only the surface properties of
Fig. 14 Main approaches for surface functionalization of nanocellulose [142].
R.K. Mishra et al.
cellulosic nanofibres without compromising the bulk charac-
teristics of nanofibres [137]. Each and every material for exam-
ple polymers, metals, or even ceramics possess a surface at the
boundary, that is connected with air or consists of an interface
where it associates another material, the chemical as well as
physical characteristics of any materials at the surface display
a big difference from its bulk chemical as well as physical char-
acteristics [6]. Consequently, the surface alteration is an excel-
lent approach to modify the functional features of materials by
tuning their surface characteristics. A similar principle is
appropriate in the matter of nanocellulose, its hydrophobicity,
as well as hydrophilicity, are tuned by adjusting the surface or
the interface of nanocellulose [66].
6. Surface modification of nanostructured cellulose
Substantial strength, extensive accessibility, minimal abrasive-
ness, renewability, light-weight, higher aspect ratio and high-
quality dimension stability are the primary advantages of
nanocellulose. Because of the hydrophilic character of cellu-
lose, NFC is never uniformly distributed as well as dispersed
in the majority of non-polar polymer medium and its suspen-
sion is a gel-like configuration at very low concentration and
NFC type films or aggregates are very soon dried [138]. Con-
sequently, NFC modification is of great interest in an effort
to reduce this phenomenon as well as open-up cutting-edge
applications. nanocellulose dependent composites exhibit com-
patibility issue between nanocellulose and nonpolar polymer
matrices. Compatibility with a larger range of matrices
employed in coating colours or in extrusion has been carried
out [6]. To develop the compatibility between nanocellulose
as well as polymer matrices, surface modification of nanocellu-
lose materials are carried out, to enhance the compatibility,
dispersibility as well as the overall performance of the
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 963

Table 10 An overview of nanocellulose fictionalization.

Type of functionalization
Molecular Functionalization
Macromolecular Functionalization
Functionalization of inorganic compounds
Remarks Ref.
 Nanocellulose -Sulfoxide functionalization [143–146]
 Nanocellulose-Amide functionalization
 Nanocellulose -Silane functionalization
 Nanocellulose-Acetyl functionalization
 Nanocellulose-Carboxylic functionalization
 Nanocellulose-Aldehyde functionalization
 Nanocellulose-Hyroxyapatite functionalization
 Nanocellulose-Epoxy functionalization [147,148]
 Nanocellulose-Cellulose Derivatives functionalization
 Nanocellulose-Polysulfone functionalization
 Nanocellulose-Polypropylene functionalization
 Nanocellulose-Polylactic Acid functionalization
 Nanocellulose-Polyurethane functionalization
 Nanocellulose-Chitosan functionalization
 Nanocellulose-Titanium Oxide functionalization [149–152]
 Nanocellulose-Fluorine functionalization
 Nanocellulose-Gold functionalization
 Nanocellulose-Silver functionalization
 Nanocellulose-Pd functionalization
 Nanocellulose-CdS functionalization

nanocellulose structured composites system. There are several
ways to change the surface of nanocellulose particularly modi-
fication of nanocellulose by utilizing the polymer, chemical
procedure, nanoparticles, employing an organic or even inor-
ganic surfactant, biochemical procedure, as shown in Fig. 14
[139–141]. These types of methods are altered and tuned either
(i) by physical interactions or adsorption of molecules or
macromolecules onto their surface or (ii) through the use of
a chemical strategy to attain covalent bonds between cellulosic
substrates and the grafting agent. The important use of func-
tionalized nanocellulose is the wastewater treatment, biomedi-
cal applications, biosensor as well as bioimaging, catalysis and
so on. Each strategy is detailed but as, a starting point [14],
Table 10 provides a summary of most reagents employed for
physical adsorption, as well as molecules or polymers grafted
at the surface of nanofibrillated cellulose (NFC).
Table 11 compares the information of chemical surface
changes onto nanofibrils cellulose. They all are extremely
recent and also some of them have already been described over
the several past years. Without a doubt, nanofibrils cellulose
generation has obviously advanced in the course of the past
few years.
7. Characterization of nanocellulose
With the help of advancements in the vast field of analytical
techniques as well as nanotechnology, scientists and experts
have described more on the topic of nanocellulose characteri-
zation. The characterization of nanocellulose is an important
argument. The principal analytical methods for the character-
ization of nanocellulose involve microscopy, spectroscopy as
well as thermal and rheological techniques [161]. These types
of characterizations are primarily applied: (i) to figure out
the nanocellulose morphology ; (ii) to examine the various fea-
tures of nanocellulose (e .g . mechanical characteristics, optical
characteristics, liquid crystallinity), and (iii) to examine the
surface of modified nanocellulose. We understand that
nanocellulose exhibits variety in its morphology with regards
to the source of extraction. Atomic force microscopy, scanning
electron microscopy, transmission electron microscopy
(TEM), nuclear magnetic resonance, dynamic light scattering,
small-angle neutron scattering, small-angle X-ray scattering,
wide-angle X-ray scattering, are the analytical techniques that
are employed to examine the morphology of the nanocellulose.
Taking into account the transmission electron microscopy,
high-resolution transmission electron microscopy (TEM) is
feasible to identify particular nanocellulose, which permits
the analysis of their sizes and shape [85]. Bringing together
the atomic force microscopy (AFM) with spectroscopic tech-
niques, the scientists and experts have examined the morphol-
ogy as well as the mechanical aspect of nanocellulose. Raman
spectroscopy can be used for calculating the crystallinity as
well as the structure of nanocellulose [162–167]. It has been
seen that classes and sources of acid hydrolysis for developing
nanocellulose may also affect the crystallinity of nanocellulose.
Scattering methods are employed to examine the polyelec-
trolytic behaviours of nanocellulose based materials. These
types of methods comprise of ultra-small-angle X-ray scatter-
ing (USAXS), small-angle X-ray scattering (SAXS), static light
scattering (SLS) as well as dynamic light scattering (DLS)
[168,169]. In addition, the hydrodynamic properties of
nanocellulose are associated with size as well as length distri-
bution of the particles in suspensions. The rheological beha-
viour of nanocellulose suspension is complex because of the
effect of liquid crystallinity and polyelectrolytic nature. At
the lower concentrations, nanocellulose suspensions in the
dilute regime display shear thinning behaviour and this beha-
viour is dominated by raising the concentration [44].
7.1. Microstructure of nanocellulose
Based on the method to obtain the nanocellulose along with
the procedure for the production of nanocellulose, a CNF
exhibits comparable morphologies in several nm dimensions.
 964
Table 11 All physical and chemical strategies used to impart grafting onto Nanocellulose.
Origin of cellulose Type of Pre- Reagent Process and solvent Remarks Ref.
treatment
Softwood bleached Kraft pulp TEMPO oxidation Cetyltrimethylammonium Mixing The degree of substitution = [63]
method bromide/didodecyl ammonium bromide/ 0.08–0.27, Surface adsorption
dihexadecyl ammonium bromide
surfactant
Sulfite softwood dissolving pulp Carboxy- Polydiallyldimethylammonium chloride/ Layer-by-layer Surface adsorption [153]
methylation Polyethylenimine/Polyhydroxyalkanoate assembly
Sulfite softwood dissolving pulp Carboxy- Perfluoro-octadecanoic acid Coating on films Surface adsorption [154]
methylation
Softwood bleached Kraft pulp TEMPO oxidation Cetyltrimethylammonium bromide Coating on films Surface adsorption [155]
surfactant
Sweden Domsjö Pulp Enzyme Acetic BmimPF6 Ionic The degree of substitution = 0.3, [156]
liquid Molecule chemical grafting
Sweden Domsjö Pulp Enzyme Butyric BmimPF6 Ionic The degree of substitution = 0.3, [156]
liquid Molecule chemical grafting
Sweden Domsjö Pulp Enzyme Iso-butyric BmimPF6 Ionic The degree of substitution = .2, [156]
liquid Molecule chemical grafting
Sweden Domsjö Pulp Enzyme Hexanoic anhydride BmimPF6 Ionic The degree of substitution = 0.3, [156]
liquid Molecule chemical grafting
Bacterial Cellulose Acetobacterxylinum Acetic anhydride Acetic acid + The degree of substitution = [157]
toluene 0.04–2.77, Molecule chemical
grafting
Bacterial Cellulose Acetobacterxylinum Acetic anhydride Acetic acid + The degree of substitution = [158]
toluene 0.15–1.76, Molecule chemical
grafting
Kenaf Bast Fibers Acetylation Acetic anhydride Pyridine The degree of substitution = [159]
1.07, Molecule chemical grafting
Bleached Eucalyptus fibres Enzyme n-octadecyl isocyanate Toluene The degree of substitution = [160]
0.09, Molecule chemical grafting
Bleached sulfite softwood dissolving pulp Carboxy- PCL-Sn(Oct)2-catalyzed ring-opening Toluene The degree of substitution = [68]
methylation polymerization 0.0Yied = 89, 16%–19%–21%,
Polymer grafting

R.K. Mishra et al.

Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 965

nanofibrils displayed three primary weight loss zones. The pre-

Table 12 Typical nanocellulose morphology with respect to
liminary weight is a result of moisture evaporation and then
their sources.
thermal depolymerization of hemicellulose additionally the
Source Nanocellulose morphology Ref. cleavage of glycosidic linkages of cellulose [182]. The broad
Wheat straw fibre Cellulose nanofibre having [170] peak in the part from 200 °C to 500 °C is because of residual
diameter 10 to 80 nm. lignin components. A convection drying of cellulose nanofib-
Kenaf bast Cellulose nanofibre having [171] rils eliminates water, gradually leading to the creation of
diameter 2–6 nm aggregates. As a result, the dried cellulose nanofibrils offer
Wood Cellulose nanofibre having [172] the lesser level of thermal stability in comparison with the orig-
diameter 15 nm inal fibres [183].
Bagasse Cellulose nanofibre having [173]
diameter 5–15 nm
Soy hulls Cellulose nanofibre having [174] 7.3. Degree of polymerization of nanocellulose
diameter 20–120 nm
Rice straw Cellulose nanofibre 4–13 nm [175] The degree of Polymerization is highly linked to the aspect
Soybean stock Cellulose nanofibre 50–100 nm [173] ratio of the nanofibres. As described earlier, any kind of pre-
Cotton Cellulose nanofibre 10– 25 nm [176] treatment method additionally decreases the degree of poly-
Empty fruit bunch Cellulose nanofibre 10–30 nm [177] merization [184]. However, the mechanical attributes of
cellulose nanoparticles rely on morphology, geometrical
shapes, crystal configuration, crystallinity, as well as the
Usually, a CNF as well as a CNC possess common diameters method employed to generate cellulose nanocrystals and cellu-
of 2–100 nm and between 2 and 30 nm, respectively, as pre- lose nanofibrils [19]. For example, the degree of polymeriza-
sented in Table 12. tion of softwood is 2249; however, the degree of
Experts mentioned the effect of solvent exchange on NFC polymerization of sulfated cellulose nanofibrils is 825 [185].
sylilation. Dimethylacetamide, as well as toluene, had been
employed in the role of solvent for the chemical surface mod- 7.4. Irreversible agglomeration effect of nanocellulose
ification. It appears that cellulose surface variation can be
accomplished based on the solvent utilized in order to reduce
Nanoparticles have problems with clustering either through
its free surface energy. The available hydroxyl active groups
aggregation (irreversible) or agglomeration (reversible) tenden-
produce the high surface free energy of the cellulose surface.
cies. Drying of particular nanocellulose produces irreversible
This particularly latest paper introduced an explanation
agglomeration disturbing their dimension and, consequently,
regarding OH availability at the surface of the NFC based
their particular extraordinary properties [186]. This irreversible
on the solvent method (Fig. 15).
agglomeration is called hornification and is connected to the
The morphology of cellulose nanocrystals (CNCs) obtained
hydrogen bonds established. When freeze-drying or even
by acid-hydrolysis from sugarcane bagasse in the role of agro-
supercritical dying with CO2 is employed, agglomeration is
waste has been discussed. The CNCs obtained by acid-
prevented [187].
hydrolysis of the CPC fibres is demonstrated in Fig. 16a.
Fig. 16(b) and (c) display the TEM as well as AFM micro-
graphs of an extremely dilute suspension of CNCs exhibiting 7.5. Film formation properties of nanocellulose
agglomerated ‘rod-like’ nanocrystals. The diameter of
nanocrystals possesses a wide range of distribution, however, Nanocellulose gels may be watered down, in addition to cast
the dimensions of the majority of the ‘rod-like’ nanocrystals or vacuum filtered and then drying to develop rigid films as
is within the range 250–480 nm in length as well as 20–60 nm a result of the development of an interfibrillar hydrogen bond-
in diameter. Their small agglomeration of CNCs reveals that ing network [188]. For example, cellulose nanofibrils films
cellulose chains offer an intermolecular hydrogen bonding achieved from sugar beet possess values of tensile strength as
along with a hydrophilic interaction between the cellulosic well as modulus of 104 MPa and 3 .5 GPa, respectively [189].
chains [179].
7.6. Surface area of nanocellulose
7.2. Thermal properties of nanocellulose
Nanocellulose possesses an excellent specific surface area. Gen-
The thermal degradation of lignocellulosic materials starts erally, cellulose nanoparticles hold SSA in the range of 50 to
with an initial decomposition of hemicelluloses, accompanied 200 g/ m2. Alternatively, nanocellulose aerogels possess speci-
by an initial phase of pyrolysis of lignin, depolymerization, fic surface area from 250 to 350 m2/g as well as have an extre-
effective flaming combustion, as well as char oxidation. Addi- mely low density (0 .02 g/cm3) and a substantial porosity of
tionally, cellulose nanofibrils consist of a very high degrada- 98% [190]. Considering the case of cellulose nanocrystals, in
tion temperature onset (350 °C) and also much better the event that cellulose nanocrystals have been completely
thermal performance compared to hemicellulose, pectin, and dried or dried significantly above its critical concentration,
lignin. On the other hand, the onset of the thermal degradation particle aggregation takes place, resulting in a reduction of fea-
of nanocrystals usually takes place at 200–300 °C [180,181]. tures as well as functionality. To eliminate this issue, surfac-
Cellulose nanocrystals with lesser sulfate amount possess more tants or surface modification can be employed to avoid
beneficial thermal stability. Alternatively, banana cellulose aggregation throughout drying [1].
966 R.K. Mishra et al.

Fig. 15 AFM and XPS data for neat and silylated NFC, in DMA and toluene [178].

Fig. 16 Morphology and topography of cellulose nanocrystals: (a) field emission-scanning electron micrograph (FE-SEM, 500 nm
scale); (b) transmission electron microscopy image (TEM, 500 nm); (c) Atomic Force Microscopy (AFM, 2 mm scale) [179].
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect
7.7. Crystallinity of nanocellulose
Crystallinity is incredibly influenced by the lignocellulosic
source. For example, crystallinity of flax, rutabaga, as well
as wood cellulose nanofibres are 59%, 64%, and 54%, respec-
tively, however, a crystallinity of 85 .9%, 76%, 84 .9%, 94%,
80 .6%, and 81 .7% had been basically noticed for cellulose
nanocrystals achieved from sisal, rice husk, flax, cotton, corn
stover, and commercial microcrystalline cellulose, respectively
[174]. Alternatively, degrees of crystallinity of 78% and also
70% have been found for wheat straw and soy hull cellulose
nanofibrils, respectively. In-depth, really low values have been
seen for beet pulp  30–40% [134]. The degree of crystallinity
levels in the sequence: pineapple > banana > jute, which
order confirms with the values of cellulose content identified
through these samples. Generally, cellulose nanocrystal that
is made from H2SO4 possesses lesser crystalline values com-
pared to those made from HCl. Also, the increase in hydrolysis
time period improves crystallinity a result of the removal of
amorphous regions [191].
7.8. Oxygen barrier properties of nanocellulose
The oxygen transmittance rate of cellulose nanofibres at 0%
relative humidity is within the range 17–18 mL/m2/day. The
improvement of relative humidity enhances the oxygen perme-
ability as a result of the constrained hydrogen bonding as well
as loose networks as water molecules enter [192,193]. The
water as well as oxygen permeability diminished with expand-
ing film thickness by reason of the insufficient interconnectivity
of pores [190]. It has been additionally seen that the applica-
tion of microfibrillated in form of a surface layer on paper
sheet decreased its oxygen permeability. It had been ascribed
to the dense configuration established by the microfibrils lead-
ing to decreased sheet porosity [194].
7.9. Rheological characteristics of nanocellulose
Cellulose nanofibres suspensions manifest a shear-thinning
tendency as well as pseudoplasticity, which often is dependent
upon the pH environment [195,196]. Sulfate cellulose displays
a pH-dependent viscosity profile as a consequence of electro-
static interactions. Furthermore, a cellulose nanofibres suspen-
sion possesses a reducing viscosity with enhancing shear rates
[197]. Additionally, CNF also provides an excellent elastic
modulus owing to the entangled network configuration [198].
7.10. Permeation properties of nanocellulose
Vapor barriers restrict the quantity of water vapour passing
throughout the structure due to distinct vapour pressures. A
vapour barrier is used to limit the circulation of water vapour
throughout a material [199,200]. As a vapour barrier, they are
able to regulate the rate of moisture flow in which they are
located. Permeance is calculated in perms. One perm is defined
as one grain of water vapour per hour pass through one square
foot of a layer, induced by a vapour pressure difference of one
inch of mercury across the two surfaces [201]. Permeability is a
characteristic of a material. Permeance is dependent upon the
thickness of the material and consequently is a capabilities
assessment and not a characteristic of a material [202].
967
Cellulose nanofibrils have the ability to build films with mini-
mal moisture diffusivity because of a stiff fiber network and,
consequently, possess outstanding barrier characteristics. The
water vapor intake rate of cellulose nanofibrils films is 20%
lesser compared to those composed of microfibers (in the range
20%–30%) [203–205]. In addition to, cellulose nanocrystals
films are anticipated to offer an excellent barrier to water
molecules because cellulose nanocrystals films hold an even
more crystalline nature as compared to cellulose nanofibrils
[190]. The water vapor transmission rate of cellulose nanocrys-
tals reinforced glycerin plasticized carboxymethyl cellulose
(CMC) films was found to decrease slightly upon heat-
treatment. Cellulose nanoparticles prepared by drop-wise
addition of ethanol/HCl aqueous solution into a NaOH/
urea/H2O suspension of micro crystalline cellulose were found
to decrease the water vapor permeability of glycerol plasti-
cizedstarch films [194,206–208].
7.11. Toxicity effect of nanocellulose
Cellulose nanocrystals carry lesser toxin level as well as mini-
mal environmental hazard based on ecotoxicological assess-
ments with a number of aquatic breeds (e .g., Daphnia,
rainbow trout as well as fathead minnow) [209,210]. Addi-
tional, cytotoxicity (intracellular poisonous consequence) and
also proinflammatory reaction are considerably less than those
for multiwalled carbon nanotubes and also crocidolite asbestos
fibers [211]. Cellulose nanofibrils reveal absolutely no side
effects as well as genotoxicity in vitro. The toxin levels of bac-
terial cellulose nanofibres have been effectively examined
in vitro via cell viability and also flow cytometric assays along
with in vivo choosing mice surgeries [212]. Also, bacterial cel-
lulose exhibits absolutely no side effects in the human being
umbilical vein endothelial cell culture, fibroblasts, as well as
chondrocytes. The in vitro analysis additionally reveals that
95% of the mesenchymal stem cells accumulate to cellulose
membrane [213].
7.12. Mechanical properties of nanocellulose
By applying nanomaterials in form of fillers in composite
materials enhanced rigidity, durability, resilience, barrier fea-
tures, and also flame retardancy can be accomplished in com-
parison to the 100% pure polymer material [214]. The
introduction of the limited proportion of nanomaterial is suf-
ficient for these enhancements as a result of the huge surface
area of the nanoparticles. In comparison to carbon nanotubes,
cellulose nanofibres from wood have only quarter of the
strength, however, the pricing with regard to cellulose nanofi-
bres are cheaper than the prices for carbon nanotubes, that
Table 13 Mechanical properties of different reinforcement
materials.
Material Tensile Elastic Ref.
strength (GPa) modulus (GPa)
Cellulose nanocrystals 7.5–7.7 110–220 [216]
Kevlar 3.5 124–130 [217]
Steel wire 4.1 210 [150]
Carbon fiber 1.5–5.5 150–500 [150]
968
makes the wood-based nanomaterial more appealing for speci-
fic applications. The strengthening capability of the cellulose
whiskers originates from its excessive surface area as well as
excellent mechanical characteristics [215]. Table 13 displays
the tensile strength as well as elastic modulus of certain distinct
types of reinforcement materials.
7.13. Biodegradability of nanocellulose
An important benefit of environment-friendly composites
which are dependent on biopolymers is their intrinsic
biodegradability. Nevertheless, a large number of artificial
biopolymers demand energy-intensive composting tempera-
tures (60 °C) for biodegradation to happen swiftly [218].
Conversely, indigenous cellulose, as well as regenerated cellu-
lose, are able to degrade quickly at surrounding temperatures
(i .e . 20–30 °C) because of the hydrophilicity of cellulose [219].
8. Application of nanocellulose
In recent times, the applications of nanocellulose have already
been mentioned extensively. The primary reality is that
nanocellulose is generally obtained from waste fruits, plant
fibres, that are obtainable in the tremendous amount. Because
of this, experts concentrate their attention in the direction of
the extraction, characteristics, as well as the application of
nanocellulose [66].
8.1. Barrier for liquid and gaseous materials
Micro as well as nano-fibrillated cellulose-based polymer film
provide decent barrier features, which is dependent upon the
fibrils morphology of cellulose, mainly because fibril morphol-
ogy behave as barrier for the penetration as well as diffusion of
liquid and even gaseous materials into the cellulose-based film
[220–222]. Fibrils morphology additionally improve the pene-
tration as well as diffusion length, which improve the barrier
attributes of polymer film [223]. Fig. 17 demonstrates the bar-
rier attributes of the nano cellulose-containing polymeric film.
8.2. Biomedical application
Biomedical topic is known as one of main area, in which
nanocellulose is being commonly used as a consequence of
its cheap production costs, accessibility, sustainability, excel-
lent mechanical properties, huge specific surface area, feasible
chemical modifications, and biocompatibility, together with
absence or unavailability of toxicity [224,225]. Nanocellulose
membrane is likewise a rising material for cell attachment as
well as proliferation due to its 3D network, excessive porosity
Fig. 17 Barrier features of nanocellulosebased polymeric film.
R.K. Mishra et al.
in addition to lower cytotoxicity. Nanocellulose membrane
carries the substantial water-holding capability, superior flexi-
bility, conformability, and excellent mechanical durability,
rendering it an appropriate aspirant for wound- dressing
[226,227]. Along with it, the cell attachment is enhanced by
the surface modification of cellulose. The modification of
nanocellulose is achieved by numerous ways, for example, pro-
tein coatings, plasma treatment method, an introduction of
surface charges and so on [66]. In the modern era, nanocellu-
lose structured drug delivery systems have been adapted to reg-
ulate the drug-release rates and subsequent drug levels.
Nanocellulose based upon hydrogel is an additional vital arti-
ficial material for biomedical use. The nanocellulose-based
hydrogel has been employed in the role of a drug carrier for
inserting various kinds of drugs [66]. It is observed that inter-
actions between the drugs together with nanocellulose perform
a vital role to produce drug stability as well as releasing the
drug. Nanocellulose based composites including antimicrobial
agents (e.g. silver nanoparticles, lysozyme) deals the antimicro-
bial special effect, as presented in Fig. 18 [228].
8.3. As reinforcement in polymer matrix
Composite materials are commonly preferred in lots of differ-
ent applications these days and are comprised of a polymeric
matrix including a filler material in the role of reinforcement.
The fillers employed are usually artificial, for example, glass
fiber, carbon, or aramid [230]. The inclusion of filler to a poly-
meric material boosts the mechanical as well as thermal char-
acteristics of the composite material, in comparison to the
polymeric material alone, due to their excellent performance
and terrific adaptability [231–233]. These days, there is cer-
tainly a substantial focus on climatic issues and the artificial fil-
lers employed in composite materials since they lead to
problems at the end-of-life disposal because of their limited
combustibility along with the high requirement on methods
for reusing the materials. By exchanging the artificial fillers
with natural types, for example, cellulose fibers, starch, or
chitin, there will be a lot of beneficial environmental positive
aspects and positive aspects such as lesser costs, lesser density,
excellent thermal properties, as well as biodegradability
[219,234]. Both cellulose nanofibrils as well as cellulose
nanocrystals equally improved mechanical as well as thermal
properties in contrast to the unfilled polymer matrix. The
strengthening effect for nanocellulose fillers takes place most
likely from the cellulose hydrogen bonding network within
the polymer matrix [14]. Between the two distinct nanocellu-
lose fillers, cellulose nanofibrils revealed the most significant
enhancement in mechanical as well as thermal performance
as a result of its morphology. A lot more flexible and hairy
nanofibrils displayed a tangling effect in comparison to the
additional specific cellulose crystals. Increased thermal charac-
teristic for cellulose nanofibrils composites from potato pulp as
well as eucalyptus pulp has additionally been discussed [235].
The combination of various types of matrix and nanocellulose
is presented in Table 14.
8.4. Nanocellulose for water purification
Membranes coupled with filters are generally employed to
remove various chemical substance by letting certain species
Materials chemistry and the futurist eco-friendly applications of nanocellulose: Status and prospect 969

Fig. 18 Biomedical applications of nanocellulose [229].

Table 14 Various types of cellulose sources in the role of reinforcement in polymer matrices.
Type of source Type of nanocellulose Type of polymer matrix References
materials
Potato pulp Cellulose nanofibrils Starch/glycerol (0–40 wt% filler) [236]
Rutabaga Cellulose nanofibrils Polyvinyl alocohol (PVA) (10 wt% filler) [237]
Microcrystaline Cellulose nanocrystals Polylactic acid (PLA) (5 wt% filler) [238]
cellulose
Hemp Cellulose nanofibrils Polyvinyl alocohol (PVA) (10 wt% filler) [237]
Bacteria Cellulose nanocrystals Cellulose acetate (CAB) (0–10 wt% filler) [239]
Cotton Cellulose nanocrystals Polyvinyl alocohol (PVA) (0–12 wt% filler) [240]
Ramie Cellulose nanocrystals Starch/glycerol (0–40 wt% filler) [112]
Tunicate Cellulose nanocrystals Styrene/butyl acrylate (6 wt% filler), Starch/sorbitol (25 wt% filler) [241]
Waterborne epoxy (0.5–5 wt% filler)
– Core-shell amylopectin-coated Starch [242]
cellulose nanofibres
Sisal Cellulose nanowhisker Polyvinyl acetate [243]
– Cellulose nanofibrils Epoxy [244]
Microcrystalline Cellulose whiskers Polylactic acid [245]
cellulose
Palm tree Cellulose nanofibrils Natural rubber [246]
Palm tree Cellulose nanocrystals Natural rubber [246]
– Cellulose nanocrystals(0–2 wt%) Poly (vinyl alcohol)(PVA) foams [247]
– Cellulose nanocrystals Polylactide [248]
Cellulose nanofibrils(0 to 10 wt%) Poly (acrylic acid-co-acrylamide) [249]
970
to cross although some other is prevented. The selectivity of a
membrane is linked to the microstructure as well as chemical
composition of the membrane material [250]. Membranes are
developed with well-defined pores for dimensions exclusion
along with a customized surface chemistry in an effort to selec-
tively adsorb certain solutes. Nanocellulose is an effective
bioadsorbent that has an excellent strength as well as versatil-
ity [251,252]. Organic contaminants in drinking water symbol-
ize a significant number of substances such as dyes, natural
oils, chemical pesticides, and also synthetic medicines materi-
als. Nanocellulose with ionic as well as non-ionic surface active
groups have likewise been applied to adsorb natural impuri-
ties, for example, dyes, natural oils, as well as chemical pesti-
cides, from aqueous solutions. Nanocellulose with cationic or
perhaps anionic surface groups are being demonstrated to
eliminate heavy metal contaminants from aqueous solution
[6,66,253]. The surface functionality of nanocellulose along
with its capability to develop mechanically durable smooth
film has been used to produce membranes for water filtration.
Various coating techniques, electrospinning, Vacuum purifica-
tion, can be employed widely to generate membranes [253,254].
Nanocellulose-based membranes in addition to filtration sys-
tems are in fact important, however, issues associated such
as cheap upscaling, biofouling, and also drawbacks in particu-
lar absorption should be resolved. Designing economical pro-
cessing techniques of surface customized nanocellulose would
be essential for the industrial execution of nanocellulose-
based membranes as well as filtration systems [254,255]. In
fact, various factor such as cost- together with highly efficient
handling as well effective utilization of membranes is impor-
tant for the future market perception of this modern technol-
ogy. Even though modified nanocellulose usually show
uptake capabilities are similar or much better than traditional
adsorbents. There is certainly a necessity to deal with some
obstacles such as the selectivity in the complicated water flows.
This tends to call for the inclusion of more precise as well as
particular surface functionalities [256,257]. Techniques
employed in the polymer membrane area can offer much more
information on the functionality of nanocellulose-based mem-
branes in genuine commercial applications. Analysis endeav-
ours to enhance the knowledge on membrane fouling,
recycling, as well as regeneration have to be executed. The sub-
sequent stage of the nanocellulose based water filtering mem-
brane system is predicted to concentrate on hybrid
membranes wherein nanocellulose is employed along with
other nanoparticles to enhance mechanical durability, pore
morphology, as well as adsorption ability [5,258,259]. In- situ
functionalization of membranes and also 3D printing will
likely allow the improved and maximum utilization of nanocel-
lulose membranes/filters in water filtration system [259–261].
9. Conclusion
This review article explains the fundamental, properties, char-
acterization and potential application of the nanocellulose.
The application of nanocellulose in the way of life has been
profitable in fields of practical application particularly as a
product packaging, papers as well as paperboard, food prod-
ucts factory, health care and additionally sanitation products,
paints, cosmetics, and so on. The various processing proce-
dures for nanocellulose have already been fully optimized for
R.K. Mishra et al.
many years, and good strategies that possibly focus on a more
significant scale are being established. For bacterial cellulose,
there is a vested interest to produce a synthesis method which
can be ideal for much larger level manufacturing, however, the
method nowadays is too costly and also requires quite a long
time. The commercialization of nanocellulose is not still com-
pletely established, but still, there are companies in addition to
preliminary crops spread in various areas on the planet supply-
ing nanocellulose for scientists and the commercialization of
the items. Different processing strategies were shortly dis-
cussed. The methods utilized rely upon kind of nanocellulose
and cellulose source. The inclusion of minimal weight amount
of nanocellulose to a polymer matrix could enhance the
mechanical features of the material, in comparison to plain
polymer matrix alone. To sum up, nanocellulose, in a number
of diverse forms, reflects growing involvement in the company
and modern society because of its several positive aspects,
which include acting as environmental friendly material, less
expensive, and substantial mechanical capabilities. Addition-
ally, nanocellulose based materials are going to take a signifi-
cant role in the future nano area.
Acknowledgements
Visvesvaraya Research Fellowship (Department Information
and Electronics, Govt. of India)
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