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Cellulose nanocrystals: synthesis, functional

properties, and applications

Johnsy George & SN Sabapathi

To cite this article: Johnsy George & SN Sabapathi (2015) Cellulose nanocrystals: synthesis,
functional properties, and applications, Nanotechnology, Science and Applications, , 45-54,
DOI: 10.2147/NSA.S64386

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Cellulose nanocrystals: synthesis, functional

properties, and applications

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4 November 2015
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Johnsy George Abstract: Cellulose nanocrystals are unique nanomaterials derived from the most abundant
SN Sabapathi and almost inexhaustible natural polymer, cellulose. These nanomaterials have received signifi-
cant interest due to their mechanical, optical, chemical, and rheological properties. Cellulose
Food Engineering and Packaging
Division, Defence Food Research nanocrystals primarily obtained from naturally occurring cellulose fibers are biodegradable and
Laboratory, Siddarthanagar, renewable in nature and hence they serve as a sustainable and environmentally friendly material
Mysore, Karnataka, India
for most applications. These nanocrystals are basically hydrophilic in nature; however, they can
be surface functionalized to meet various challenging requirements, such as the development
of high-performance nanocomposites, using hydrophobic polymer matrices. Considering the
ever-increasing interdisciplinary research being carried out on cellulose nanocrystals, this review
aims to collate the knowledge available about the sources, chemical structure, and physical and
chemical isolation procedures, as well as describes the mechanical, optical, and rheological
properties, of cellulose nanocrystals. Innovative applications in diverse fields such as biomedical
engineering, material sciences, electronics, catalysis, etc, wherein these cellulose nanocrystals
can be used, are highlighted.
Keywords: sources of cellulose, mechanical properties, liquid crystalline nature, surface
modification, nanocomposites

Introduction
Cellulose is the most abundant natural polymer available on the earth and it is an
important structural component of the cell wall of various plants. Apart from plants,
cellulose is also present in a wide variety of living species, such as algae, fungi, bac-
teria, and even in some sea animals such as tunicates.1 Cellulose is a fibrous, tough,
and water-insoluble polymer and it plays an essential role in maintaining the structure
of plant cell walls. Moreover, cellulose is a biodegradable, biocompatible, and renew-
able natural polymer and hence it is considered an alternate to nondegradable fossil
fuel-based polymers. The chemical structure of cellulose (Figure 1) shows that the
polymer, formed by condensation, consists of monomers joined together by glyco-
sidic oxygen bridges. Cellulose is composed of β-1,4-linked glucopyranose units that
form a high–molecular-weight linear homopolymer, in which every monomer unit is
corkscrewed at 180° with respect to its neighbors.2 The repeating unit of this natural
polymer is a dimer of glucose, known as cellobiose. The degree of polymerization of
Correspondence: Johnsy George
Food Engineering and Packaging Division,
cellulose can vary depending on the source and it is approximately 10,000 glucose
Defence Food Research Laboratory, units for wood-derived cellulose and 15,000 units for cotton-derived cellulose.3 Each
Bannur Road, Siddarthanagar,
Mysore 570 011, Karnataka, India
glucopyranose unit bears three hydroxyl groups, which impart cellulose some of the
Email [email protected] characteristic properties such as hydrophilicity, chirality, biodegradability, etc, which

submit your manuscript | www.dovepress.com Nanotechnology, Science and Applications 2015:8 45–54 45
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OH OH OH
OH OH OH
HO O HO O O
HO
O O O
HO O O OH
HO HO HO
O O O
OH OH OH
OH OH OH
n

Figure 1 The chemical structure of cellulose, which is a linear polymer made up of β-D-glucopyranose units covalently linked with (1–4) glycosidic bonds.

are initiated by the high reactivity of the hydroxyl groups.1 an exceptionally high degree of crystallinity, which can be
The ability of these hydroxyl groups to form strong hydrogen as high as 95%.8 Depending on the biosynthesis process
bonds is the main reason for some other properties such as occurring in different species, the properties of cellulose
multiscale microfibrillated structure, hierarchical organi- microfibrils obtained may also differ.
zation (crystalline and amorphous fractions), and highly
cohesive nature.4 Bacteria
Certain species of bacteria, eg, Komagataeibacter xylinus,
Main sources of cellulose which occur as contaminants during vinegar fermentation, are
The main sources of cellulose are plants; however, algae, well known for producing cellulose by utilizing a large variety
bacteria, and some sea animals are also capable of producing of nitrogen and carbon sources.9 K. xylinus produces cellulose
cellulose in large quantities.5 A brief description about the microfibrils in the form of clear, flat, and thick pellicles floating
main sources is as follows. on the surface of the growth medium.10 These cellulose pellicles
comprise pure cellulose along with a large proportion of water
Plants and other ingredients of the medium. Dilute alkaline solutions
Plants are the potential main sources of cellulose because are capable of hydrolyzing and removing the impurities present
they are abundant and relatively cheap. The main source in the cellulose pellicle.11 After alkali treatment and washing, the
of cellulose is wood pulp and cotton fibers. Large-scale cellulose pellicles can be dried and processed into pure cellulose
industrial infrastructures are presently available for their membranes. Microbially derived cellulose is unique and has
harvesting, processing, and extraction. A wide variety of several advantages over plant-derived cellulose as the former
other plant materials such as jute, ramie, sisal, flax, hemp, etc possesses better properties such as 1) unique nanostructure,
are also well known sources for cellulose production.6 Other 2) purity, 3) higher-dimensional stability, 4) greater mechani-
cellulose-producing plants include water plants, grasses, cal strength, and 5) greater capacity to hold water.12 Microbial
and some parts of plants such as leaves, stem, fruit, etc. cellulose is identical to plant cellulose in terms of its molecular
Agricultural wastes such as wheat and rice straw, sugarcane formula and polymeric structure, but the two forms differ in
bagasse, sawdust, cotton stables, etc are also used for the the arrangement of glycosyl units within the unit cells of the
production of cellulose. crystallites, which leads to higher crystallinity of the former.
Compared to plant cellulose, microbial cellulose also exhibits
Algae a high degree of polymerization and superior properties.
Native cellulose is a major component of the cell wall of many
types of algae, which are highly crystalline. Various types of Tunicates
algae such as red, green, and yellow are known for cellulose Tunicates are marine invertebrate sea animals that are well
production; however, green algae are the most preferred ones known for producing cellulose in large amounts. These ani-
for cellulose extraction. Common cellulose-producing algae mals have a thick, leathery mantle, which is a good source
belong to the orders Cladophorales (Cladophora, Chaetomor- of cellulose. Cellulose acts as a skeletal structure in the tunic
pha, Rhizoclonium, and Microdyction) and Siphonocladales tissues, which is a unique integumentary tissue that covers
(Valonia, Dictyosphaeria, Siphonocladus, and Boergesenia).7 the entire epidermis of the tunicates.13 Cellulose is produced
The cellulose derived from Valonia or Cladophora possesses by these animals using enzyme complexes present in the

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Dovepress Cellulose nanocrystals

membrane of the epidermis. Large numbers of tunicate spe- When these microfibrils are subjected to a proper combina-
cies are available in nature and the properties of cellulose tion of mechanical, chemical, and enzyme treatments, the
obtained can vary from species to species. The structure and highly crystalline regions of the cellulose microfibrils can be
properties of the cellulose microfibrils obtained from differ- extracted, resulting in the formation of cellulose nanocrys-
ent species are often comparable, but small differences in the tals (CNCs).21 CNCs are stiff rod-like particles consisting
cellulose microfibril formation process may affect the final of cellulose chain segments in a nearly perfect crystalline
properties of microfibrils. structure. These nanocrystals are also referred to as whiskers,
nanoparticles, nanofibers, microcrystallites, and so on, but the
Hierarchical arrangement most widely accepted nomenclature is CNCs.2 Compared to
of cellulose bulk cellulose, which has greater amorphous fractions, these
Cellulose is synthesized as individual molecules with a long nanocrystals exhibit high specific strength, modulus, high
chain, but it undergoes spinning in a hierarchical order at the surface area, and unique liquid crystalline properties.
site of biosynthesis to form assemblies of cellulose fibers. Many Several mechanical processes, such as high-pressure
individual cellulose chains assemble together to form elemen- homogenizations, high-intensity ultrasonic treatments,
tary fibrils (protofibrils), having an approximate diameter of microfluidization techniques, cryocrushing, etc, have been
3.5 nm.14 Depending on the source, the elementary fibrils’ utilized for the extraction of cellulose microfibrils. These
diameter can vary in the range of 2–20 nm, and they are found mechanical processes produce enough shear forces to split
in different packing arrangements depending on the conditions apart the cellulose fibers along the longitudinal axis and
that govern biosynthesis. The microfibrils are formed by the help to extract the cellulose microfibrils. Each cellulose
aggregation of elementary fibrils by coalescence, which is microfibril is devoid of chain folding and can be considered
used as a mechanism to reduce the free energy of the surfaces.15 a string of cellulose crystals, linked along the microfibril by
This aggregation phenomenon is supported by van der Waals disordered or paracrystalline regions.22 The chemical method
forces, as well as intra- and intermolecular hydrogen bonds. The of converting cellulose microfibrils into CNCs is better
cellulose molecules that are aggregated to form microfibrils than the mechanical methods as the former reduces energy
have different orientations depending on the source. The micro- consumption and also produces rod-like short nanocrystals
fibril aggregates also consist of tightly packed cellulose chains with improved crystallinity. Ribbon-like nanofiber samples
that form crystallites, which are stabilized by complex and obtained from wood-derived cellulose after mechanical refin-
strong hydrogen bonds, along with some less-ordered chains ing exhibit a lower crystalline fraction (0.05–0.55) compared
that form amorphous regions.16 Depending on the inter- and to rod-like wood CNC (0.6) obtained after acid hydrolysis.23
intramolecular interactions and molecular orientations present, Strong acid hydrolysis is usually used for the removal of
cellulose can exist as different polymorphs or allomorphs. amorphous domains that are regularly distributed along
Already six interchangeable polymorphs, viz, cellulose I, II, the microfibrils. Strong acids can easily penetrate into the
IIII, IIIII, IVI, and IVII have been identified, the contents of which amorphous regions having a low level of order and hydrolyze
vary depending on the source of cellulose.17 Native cellulose them, leaving the crystalline regions unaffected.
generally has the crystal structure of cellulose I, but it is again Colloidal suspensions of cellulose were first synthesized
subdivided into allomorphs Iα and Iβ.18 Cellulose Iα possesses by Ranby24 in 1951 by using a controlled sulfuric acid-
a triclinic structure, whereas Iβ has a monoclinic crystalline catalyzed degradation of cellulose fibers. The degradation
structure.19 Cellulose obtained from microbial and algal sources induced by boiling cellulose fibers in acidic solution reached
is rich in Iα, while cellulose forming cell walls of higher plants a limit after a certain period of treatment. Transmission elec-
is rich in Iβ. These microfibrils assemble into larger units called tron microscopy and electron diffraction studies confirmed
macrofibrils, and they in turn further assemble together to form the presence of needle-shaped cellulose particles, which
the familiar cellulose fibers. possessed the same crystalline structure as the original
cellulose fibers.25,26 Acid hydrolysis of cellulose, followed
Cellulose nanocrystals by ultrasound sonication, later led to the development of
and their isolation microcrystalline cellulose.27 The differences in the kinetics of
Naturally occurring bulk cellulose consists of highly ordered, hydrolysis between amorphous and crystalline domains led to
crystalline regions along with some disordered (amorphous) the selective cleavage of cellulose chains.28 As a result of acid
regions in varying proportions, depending on its source.20 hydrolysis, a rapid decrease in the degree of polymerization

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47
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George and Sabapathi Dovepress

was observed, which reached a cutoff level known as the cellulose domains are resistant to hydrolysis for a longer time
level-off degree of polymerization (LODP). The value of compared to disordered or amorphous regions and hence, they
LODP varies depending on the cellulose origin, where cotton- can be easily separated from the acid medium. The processing
derived cellulose possesses an LODP of 250, 300 for ramie conditions used during the hydrolysis process, such as reaction
fibers, 140–200 for bleached wood pulp fibers, and up to time, the temperature used, etc, are very critical in controlling
6,000 for cellulose obtained from Valonia.29–32 CNCs obtained the yield and quality of CNCs. If the hydrolysis time is inad-
by the acid hydrolysis of cellulose from bacteria, tunicates, equate, then amorphous fractions remain, which may result in
or Valonia exhibit a high polydispersity in the molecular the reduction of crystallinity and change in particle morphol-
weight, without any evidence of the LODP, probably due ogy. Similarly, allowing the reaction to continue for a long time
to the absence of the regular distribution of the amorphous can lead to depolymerization of crystalline cellulose, which
domains. A new concept to prepare cellulose nanomaterials decreases the aspect ratio of the nanocrystals. Temperature
was reported, whereby enzymatic hydrolysis was used in is also a critical factor as higher reaction temperatures prove
combination with mechanical shearing and high-pressure to be effective in obtaining shorter CNCs.36
homogenization, leading to a controlled fibrillation down
to the nanoscale, to produce cellulose nanomaterials with a Dimensions of CNCs
diameter of ∼5–6 nm.33 Bacterial CNCs were also reportedly The geometric dimensions of CNCs, such as length and width,
isolated using a commercially available cellulase enzyme in may vary depending on the origin of cellulose microfibrils and
combination with mechanical shearing, which is depicted in the acid hydrolysis conditions such as time, temperature, purity,
Figure 2.34 The nanocrystals prepared by this route exhibited etc. CNC exhibits a relatively broad distribution in length and
better mechanical and thermal properties as compared to the width because of the diffusion-controlled nature of the hydroly-
nanocrystals obtained from sulfuric acid hydrolysis. sis process. The dimensions of CNCs depending on the source
Prolonged hydrolysis can lead to further reduction in the and preparation method are summarized in Table 1.
molecular weight, and hence, to obtain CNCs, acid hydrolysis The average length of the rod-shaped particle can vary
has to be stopped after attaining LODP.35 Highly crystalline from tens of nanometers to several micrometers, while width
ranges from 3 nm to 50 nm. CNCs obtained from wood were
reported to have diameter and length in the range of 3–5 nm and
100–300 nm, respectively.37 CNCs obtained from cotton were
found to have diameter of 5–10 nm and length of 100–150 nm,
while that of Ramie is 70–200 nm and 5–15 nm, respectively.38,39
Similarly CNC from sisal exhibited length in the range of
100–300 nm and diameter in the range of 3–5 nm.40 Sea algae,
such as Valonia ventricosa, produce CNCs having dimensions
in the range of 20 nm diameter and 1,000–2,000 nm length,
while sea animals such as tunicates produce nanocrystals with
10–20 nm diameter and 500–2,000 nm length.41,42 CNCs pro-
duced from bacterial cellulose by HCl hydrolysis were found
to have their diameter and length in the range of 10–20 nm and
100–300 nm, respectively, while H2SO4 hydrolysis, produced
bacterial CNC with a higher aspect ratio.43,44 The geometrical
aspect ratio of CNCs, which is the ratio of length to diameter
(L/D), is very important in defining the reinforcing capability
of CNCs. CNCs having a high aspect ratio generally show bet-
Figure 2 Bacterial cellulose nanocrystals isolated using a commercially available ter reinforcing ability. The aspect ratio also plays an important
cellulase enzyme in combination with mechanical shearing. role in the formation of percolated networks that improve the
Notes: AFM images of bacterial cellulose fibers (A), bacterial cellulose fibers after
mechanical disintegration (B), bacterial cellulose nanocrystals obtained by enzyme mechanical performances of polymer nanocomposites.45
treatment after 12 hours (C) and debris obtained after complete hydrolysis (D).
Reprinted from George J, Ramana KV, Bawa AS, Siddaramaiah. Bacterial cellulose
nanocrystals exhibiting high thermal stability and their polymer nano­composites. Properties of CNCs
Inter J Biol Macromol, 2011;48:50–57.34 Copyright © 2011, with permission from
Elsevier Limited.
The important properties of CNCs can be described under three
Abbreviation: AFM, atomic force microscopy. main categories, which are briefly discussed as follows.

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Dovepress Cellulose nanocrystals

Table 1 Overview of the dimensions of cellulose nanocrystals depending on the source and preparation method
Source Preparation method Length (nm) Width (nm) Aspect Reference
ratio (L/D)
Wood H2SO4 hydrolysis 100–300 3–5 20–100 37,45
Cotton HCl hydrolysis 100–150 5–10 10–30 38
Ramie H2SO4 hydrolysis 70–200 5–15 ∼12 39
Sisal H2SO4 hydrolysis 100–300 3–5 ∼60 40
Valonia H2SO4 hydrolysis 1,000–2,000 10–20 50–200 41
Tunicates H2SO4 hydrolysis .1,000 10–20 ∼100 42
Bacteria H2SO4 hydrolysis 100–1,000 10–50 2–100 43
Bacteria HCl hydrolysis 160–420 15–25 7–23 44
Abbreviation: L/D, length:diameter.

Mechanical properties which can either lead to a chiral nematic or a cholesteric

The limitations in measuring the mechanical properties of phase of stacked planes aligned along a perpendicular axis
nanomaterials along multiple axes have made the quantitative depending on the concentration.46 Various factors such as size,
evaluation of the tensile modulus and strength of CNC charge, shape, dispersity, electrolyte, and external stimuli
extremely challenging. In addition to this, different factors can also affect the liquid crystallinity of CNC. The liquid
such as anisotropy, defects in the nanocrystals, percentage crystallinity of nanocrystals coupled with the birefringent
crystallinity, dimensions of the samples, and so on can also nature leads to interesting optical phenomena. The type of
affect the results. Theoretical calculations and indirect experi- acid used for hydrolysis can also affect the liquid crystalline
mental measurements using atomic force microscopy (AFM), nature. CNC obtained by sulfuric acid hydrolysis often pos-
X-ray diffraction analysis, inelastic X-ray scattering, Raman sesses a negatively charged surface, which promotes uniform
scattering, etc were used to calculate the elastic properties of dispersion in water due to electrostatic repulsions.50 Even
CNC.46 The theoretical tensile strength of CNCs was found to though the interactions between nanocrystals are strong,
be in the range of 7.5–7.7 GPa, which is much more than that highly sulfonated CNC is readily dispersible and this leads
of steel wire and Kevlar®-49.46 In another study, the elastic to the development of lyotropic behavior.51 Sulfuric acid- and
modulus of the CNC obtained from tunicates was determined phosphoric acid-derived CNCs normally give chiral nematic
using AFM, whereby the AFM tip was used to perform a structure, whereas hydrochloric acid-derived CNCs with
three-point bending test. The elastic moduli of CNCs were postreaction sulfonation give rise to a birefringent glassy
found to be ∼150 GPa.47 Using AFM, the transverse elastic phase.
modulus of CNCs was also determined by comparing the
experimental force–distance curves with three-dimensional Rheological properties
finite elemental calculations.48 This measurement proved Rheological parameters of CNC are influenced by prop-
that the transverse modulus of an individual CNC lies in erties such as liquid crystallinity, ordering, and gelation
the range of 18–50 GPa. The deformation micromechanics properties. Dilute CNC suspensions show shear thinning
analysis of tunicate cellulose whiskers using Raman spec- behavior, which shows concentration dependence at low
troscopy proved that the calculated modulus of tunicate CNC rates. At higher concentrations, in which the suspensions
is ∼143 GPa.49 are lyotropic, they exhibit anomalous behavior. The main
reason for such behavior is that the rod-shaped nanocrys-
Liquid crystalline nature of CNCs tals tend to align at a critical shear rate. As the shear rate
Under suitable conditions and at critical concentrations, all reaches a critical point, the chirality of the CNC suspension
asymmetric rod-like or plate-like particles spontaneously breaks down in favor of a simple nematic structure.52 In
form ordered structures, leading to the formation of a nematic addition, the relaxation time constant depends on the aspect
phase. Rod-like CNCs, when dispersed in water, self-align to ratio, and CNCs with higher aspect ratios stay aligned for
form chiral nematic phases with liquid crystalline properties. longer times even after shear. The type of acid used for
Their stiffness, aspect ratios, and the ability to align under hydrolysis can also influence the rheological properties
certain conditions make them ideal for exhibiting liquid crys- of CNC suspensions. Sulfuric acid-treated crystals show
talline behavior. However, cellulose crystallites are known to some shear thinning that is independent of time, while HCl-
have a helical twist down the long axis, similar to a screw, derived crystals show much higher shear thinning behavior,

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George and Sabapathi Dovepress

anti-thixotropy at lower concentrations and thixotropy at Applications of CNCs

higher concentrations.53 CNC is a suitable nanomaterial for a wide range of applica-
tions, such as enzyme immobilization, synthesis of antimi-
Surface modification of CNCs crobial and medical materials, green catalysis, biosensing,
CNCs have very high surface-to-volume ratios, as well as synthesis of drug carrier in therapeutic and diagnostic
plenty of hydroxyl groups, which make it suitable for many medicine, etc.60,61 These nanomaterials offer several potential
types of surface functionalizations. By introducing any advantages as drug delivery excipients due to their proper-
chemical functionality on their surface, the type of interac- ties such as smaller size, hydrophilicity, biocompatibility,
tions that the material exhibits with its surroundings can be etc.62 Due to their very large surface area and possibility of
modified. Commonly used surface functionalizations for acquiring negative charge during hydrolysis, large quantities
CNCs are esterification, etherification, oxidation, amida- of drugs can be bound to the surface of these materials with
tion, carbamation, nucleophilic substitution, silylation, the potential for optimal control of dosing.62 In one such
polymer grafting, etc.54 The main advantage of chemical report, CNCs prepared from softwood were used to bind
functionalization is that it can introduce either negative or ionizable drugs such as tetracycline and doxorubicin, which
positive electrostatic charges on the CNC surface, which could be released rapidly over a 1-day period.63 The abundant
ultimately provides better dispersion in any solvent/poly- surface hydroxyl groups present in nanocrystals provide sites
mer. It also helps to tune the surface energy characteristics for surface modification with a range of chemical groups.
to improve compatibility, especially when used along with Surface modification can be used to modulate the loading
nonpolar or hydrophobic polymer matrices.2 Esterification and release of drugs that do not normally bind to cellulose,
involves the conversion of the surface hydroxyls of cel- such as nonionized or hydrophobic drugs.64 CNC-based
lulose to esters. Sulfation and phosphorylation are some aerogels are also receiving growing interest in biomedical and
commonly used esterification reactions for cellulose. Ether- pharmaceutical applications due to their open pore structure
ification is another important chemical modification, and and high surface area, which can provide enhanced drug
the most common practice is to use glycidyltrimethylam- bioavailability and better drug-loading capacity.65 Highly
monium chloride or its derivatives to cationize the surface porous nanocellulose aerogel scaffolds were reported to attain
of the cellulose.55 Mild alkaline cationization conditions sustained drug release, which also revealed new possibilities
preserve the crystalline morphology and dimensions of as carriers for controlled drug delivery.66
CNCs.56 Surface-carboxylated CNCs with different sizes The utilization of CNCs for various applications can be
and degrees of oxidation were synthesized using TEMPO of two broad types: one type involves the use of functional-
(2,2,6,6-Tetramethylpiperidin-1-yl)oxyl)-mediated oxida- ized or nonfunctionalized as-synthesized CNC, and the other
tion of cotton.57 In the amidation technique, oxidized CNCs one involves the use of polymer nanocomposites wherein
were used as the starting material, whereby carboxylic acid CNC acts as a reinforcing agent. As a result of their distinc-
moieties were converted into amide products by react- tive properties, as-synthesized CNCs have the potential
ing them with a primary amine.58 Araki et al applied this for being used in various and diverse applications ranging
technique to bind poly(ethylene glycol) covalently with from products such as nanopaper, barrier films, and pH sen-
the cellulose surface and stabilized suspensions of CNCs sors, to stabilization of oil/water interfaces, to production
in various solvents were synthesized.38 In the carbamation of Pickering emulsions with outstanding stability, etc, but
reaction, isocyanates were used to modify CNCs. The sur- CNC-containing polymer nanocomposites has many more
face modification of CNCs using isocyanates was reported applications.67–70
by Siqueira et al, who modified sisal-based CNCs with A polymer nanocomposite is a multiphase material
n-octadecyl isocyanate without any catalyst.59 Silanes can wherein the polymer phase is reinforced with a nanomaterial.
also be grafted onto CNCs, which is one technique used to These polymer nanocomposites exhibit unique properties
enhance the interactions with polymer matrices. Perhaps, because of their nanometric size and the increased surface
chemical modification of CNCs is most useful in the area area of the reinforcing material. CNC is used as the load-
of fabricating polymer nanocomposite materials. However, bearing constituent in many polymer nanocomposite systems
the main challenge in this process lies in preserving the as it can produce significant improvements in mechanical
original morphology and maintaining the integrity of the properties even at very low volume fractions. Furthermore,
CNCs. its high aspect ratio, good dispersion in hydrophilic ­systems,

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Dovepress Cellulose nanocrystals

and the capability to form percolated network-type architec- Considering the biocompatibility of CNC and the possibility
ture within the polymer matrix make it a widely preferred of chemical modifications such as fluorescent labeling, CNCs
reinforcing component. In the area of polymer nanocompos- are potentially useful in the field of biomedical applica-
ites, CNCs are also used as model nanofillers with a defined tions such as biosensors, bioprobes, fluorescence bioassays,
morphology to impart sufficient strength and modulus. Both bioimaging applications, and so on.90 Fluorescently labeled
natural and synthetic polymers are used for the fabrica- CNCs enable the use of fluorescence techniques to study the
tion of nanocomposites. Several natural polymers, such as interaction between CNCs and living cells in vivo.91 CNCs
starch, chitosan, natural rubber, cellulose acetate butyrate, are also capable of forming highly functional nanocomposites
carboxymethyl cellulose, hydroxypropyl methylcellulose, for applications such as ultrathin film-coating materials.92
gelatin, and soy protein, are used in the preparation of nano- CNC can also be used for stabilizing nanoparticles of specific
composites.71–77 Similarly, several synthetic polymers such as functionality for specific applications. CNC-containing poly-
polyvinyl alcohol (PVA), polyvinyl chloride, polyethylene, mer nanocomposites is also used for developing membranes,
polycaprolactone, polypropylene, and polyurethane are also fibers, textiles, batteries, supercapacitors, electroactive
used.78–82 polymers, and sensors and actuators that utilize electrome-
The main challenge in achieving excellent performance chanical responses.93,94 One future area of application wherein
lies in attaining homogeneous dispersion of nanocrys- CNC-containing polymer nanocomposites can make an
tals within the polymer matrix and a good matrix–filler impact is in the field of biodegradable packaging materials.
interaction. Good dispersibility of the CNCs in the polymer The incorporation of CNC can significantly improve the
matrix is a prerequisite to make polymer nanocomposites mechanical performance, thermal stability, and barrier and
with better properties, as a nonhomogeneous dispersion of optical properties due to its improved crystallinity and better
the filler in the polymer matrix decreases the final mechanical interfacial interaction. Biodegradable nanocomposite films
properties of the nanocomposite material.83 CNCs can form with superior properties can also find their applications in
stable colloidal dispersions in water and hence they are best food and biomedical packaging areas, in which lower per-
suited for water-soluble or water-dispersible polymers such meability to moisture, gases, aroma, and oil are very much
as latexes. However, stable cellulose nanoparticle dispersions needed.95 In one research investigation, PVA-based barrier
in nonpolar solvents can also be obtained by using either sur- membranes containing different amounts of CNCs have been
factants or surface chemical grafting. Among these, the use of reported.96 These membranes containing up to 10 weight
the polymer grafting method is better in some cases due to the percentage of CNCs have been found to reduce the water
presence of the covalent linkage between the compatibilizer vapor transmission rate. The presence of highly crystalline
and the nanocrystal.84 In addition, if the grafted chains and the nanocrystals can increase the tortuosity of water vapor within
matrix are the same, better compatibilization can be obtained the polymer, leading to a slower diffusion process and, hence,
due to the formation of a co-continuous phase. lower permeability. The barrier properties are enhanced if the
With the help of the chemical grafting method, various filler is less permeable and has good dispersion in the matrix
functional molecules such as fluorescent molecules, DNA, along with a high aspect ratio. However, many scientific and
etc can also be attached on the surface of CNCs, which can technological challenges have to be addressed in several
be used for anchoring in a biological environment. It is also areas, such as optimizing suitable processing technologies
possible to disperse cellulose whiskers in an organic sol- for reducing the production cost, establishing the compat-
vent without either addition of a surfactant or any chemical ibility between products and packaging materials, meeting
modification.85 Moreover, in some cases, better dispersion of several packaging legislations, etc, before achieving a truly
CNCs leads to the formation of a percolated network of nano- biodegradable packaging material that satisfies both industry
crystals within the polymer matrix, which also contributes to requirements and consumer expectations.
enhancement in the properties of polymer nanocomposites.
These types of nanocomposites are used for making Conclusion
biomimetic foams, toughened paper, flexible panels for flat CNC is unique among a range of other nanostructured
panel displays, water repellents, and high-security papers.86–89 materials due to its benefits such as being a renewable, sus-
They are also useful for various biomedical applications such tainable, nontoxic, and biocompatible nanomaterial. Due to
as wound healing patches, tissue engineering scaffolds, and its nanometric dimensions, large aspect ratio, and excellent
hydrogels for clinical and pharmacological applications, etc. mechanical and chemical properties, CNC has many ­potential

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51
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George and Sabapathi Dovepress

applications in many areas, including materials science, 11. George J, Ramana KV, Sabapathy SN, Jagannath JH, Bawa AS.
Characterization of chemically treated bacterial (Acetobacterxyli-
electronics, and medicine. The emerging industrial extrac- num) biopolymer: Some thermo-mechanical properties. Int J Biol
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Cellulose: structural and functional aspects. Ellis Horwood, Chichester,
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cal, mechanical, optical, and liquid crystalline properties of 13. Zhao Y, Li J. Excellent chemical and material cellulose from tunicates:
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to manipulate the functionality of CNC without affecting its 3427–3441.
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this area may lead to versatile nanomaterials with improved 17. Brinchi L, Cotana F, Fortunati E, Kenny JM. Production of nanocrystal-
line cellulose from lignocellulosic biomass: technology and applica-
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uniform dispersion and distribution of CNC in a polymer 18. Atalla RH, Vanderhart DL. Native cellulose: a composite of two distinct
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Disclosure 23. Sacui IA, Nieuwendaal RC, Burnett DJ, Stranick SJ, Jorfi M. et al.
The authors report no conflicts of interest in this work. Comparison of the properties of cellulose nanocrystals and cellulose
nanofibrils isolated from bacteria, tunicate, and wood processed using
acid, enzymatic, mechanical, and oxidative methods. ACS Appl Mater
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