Nanocellulose-Based Polymer Hybrids and Their Emerging Applications in Biomedical Engineering and Water Purification

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Nanocellulose-based polymer hybrids and their emerging applications in

biomedical engineering and water purification
Article in RSC Advances · January 2019

DOI: 10.1039/C9RA03261D
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RSC Advances
REVIEW
Nanocellulose-based polymer hybrids and their

Cite this: RSC Adv., 2019, 9, 19143
emerging applications in biomedical engineering
and water purification
a
Dinesh K. Patel, Sayan Deb Duttab and Ki-Taek Lim *b
Nanocellulose, derived from cellulose hydrolysis, has unique optical and mechanical properties, high
surface area, and good biocompatibility. It is frequently used as a reinforcing agent to improve the native
properties of materials. The presence of functional groups in its surface enables the alteration of its
behavior and its use under different conditions. Nanocellulose is typically used in the form of cellulose
nanocrystals (CNCs), cellulose nanofibers (CNFs), or bacterial nanocellulose (BNC). CNCs and CNFs have
a high aspect ratio with typical lengths of 100–250 nm and 0.1–2 mm, respectively; BNC is
nanostructured cellulose produced by bacteria. Nanohybrid materials are a combination of organic or
inorganic nanomaterials with macromolecules forming a single composite and typically exhibit superior
optical, thermal, and mechanical properties to those of native polymers, owing to the greater
interactions between the macromolecule matrix and the nanomaterials. Excellent biocompatibility and
biodegradability make nanocellulose an ideal material for applications in biomedicine. Unlike native
polymers, nanocellulose-based nanohybrids exhibit a sustained drug release ability, which can be further
Received 1st May 2019
Accepted 29th May 2019
optimized by changing the content or chemical environment of the nanocellulose, as well as the
external stimuli, such as the pH and electric fields. In this review, we describe the process of extraction
DOI: 10.1039/c9ra03261d
of nanocellulose from different natural sources; its effects on the structural, morphological, and
rsc.li/rsc-advances mechanical properties of polymers; and its various applications.
1. Introduction
Cellulose is the most abundant polymer in nature1 and consists
of polysaccharides with long chains of b-D-glucopyranose units
a
assembled by b-1,4 glycosidic bonds, which form a dimer
The Institute of Forest Science, Kangwon National University, Chuncheon 24341,
Republic of Korea known as cellobiose.2 It is an important constituent of plant cell
b
Department of Biosystems Engineering, College of Agriculture and Life Sciences, walls, where it provides mechanical support; it is also present in
Kangwon National University, Chuncheon 24341, Republic of Korea. E-mail: ktlim@ other organisms such as bacteria, fungi, algae, and even sea
kangwon.ac.kr
Dinesh K. Patel has obtained his Sayan Deb Dutta received his
PhD degree from the Indian Master's degree from the
Institute of Technology (BHU)- University of Kalyani in 2017.
Varanasi, India in 2016. He will receive his PhD degree
Currently, He is working as under the supervision of
a postdoctoral fellow at Kang- Professor Ki-Taek Lim from the
won National University, Chun- Department of Biosystems Engi-
cheon, Republic of Korea. His neering, Kangwon National
research interests are on the University. His current research
structure–property relationships interests focus on the character-
of polymer nanohybrids, with ization of various cellulose-
recent focus on nanocellulose, based biomaterials as extracel-
and their applications. lular matrices for tissue engi-
neering applications.
This journal is © The Royal Society of Chemistry 2019 RSC Adv., 2019, 9, 19143–19162 | 19143
RSC Advances Review
Fig. 1 Chemical structure and intra, intermolecular hydrogen bonding in cellulose. Reproduced with permission from ref. 6; Copyright 2014,
Elsevier.
animals.3 Cellulose contains both disordered and ordered regions from the source materials, forming highly ordered
regions in its polymer chains and, owing to its renewability, low crystalline cellulose structures.12 Therefore, CNCs are crystalline
cost, abundance, and biodegradability, is a promising material in nature and can be used as reinforcing agents for a wide range
for biomedical applications.4 The polysaccharide chains of applications.13,14 CNFs are a different form of nanostructured
assemble to form microbrils, which, in turn, assemble to form cellulose, composed of long ber networks with typical lengths
macro bers and bers, through numerous hydrogen bonds.5 of 0.1–2 mm and diameters approximately equal or larger than
The chemical structure and intra- and inter-molecular hydrogen those of CNCs.15 CNFs contain amorphous cellulose in their
bonds in cellulose are depicted in Fig. 1.6 Nanocellulose is structure and, therefore, are not as crystalline as CNCs.7 BNC,
a form of nano-structured cellulose, which is typically used in also known as microbial cellulose, is another form of nano-
the form of cellulose nanocrystals (CNCs), cellulose nanobrils structured cellulose, which is produced by bacterial actions; It
(CNFs), or bacterial nanocellulose (BNC). CNCs, also known as has a typical cross-section diameter of 20–100 nm and a degree
cellulose nanowhiskers, are needle-like cellulose crystals with of polymerization (DP) of 4000–10 000.15 Other forms of nano-
typical widths of 10–20 nm and lengths of 100–250 nm;7 they are cellulose are amorphous nanocellulose (ANC) and cellulose
produced from several biological sources, such as wood, cotton, nanoyarns (CNY). A comparison of the these different forms of
wheat straw, rice husk, bamboo,8 potato tuber, sugar beet, nanostructured cellulose (CNC, CNF, BNC, ANC and CNY) is
ramie,6 bacteria,9 and algae,10 typically through strong acid shown in Table 1.16 The fabrication of high-performance poly-
hydrolysis.11 Acid treatments cause the removal of disordered mer materials using nanoparticles or nanollers has received
signicant attention in recent years by both academia and
industry.17 The hybrid material is a combination of an intimate
mixture of inorganic components, organic components or both
Ki-Taek Lim is an assistant
types of component.18 Polymer nanohybrids are composed of
professor of the department of
a combination of organic or inorganic nanomaterials with
biosystems engineering at Kang-
polymer matrices into a single composite. The overall proper-
won National University (KNU),
ties of nanohybrids are highly inuenced by the nature and
where he has been since
interactions of the nanomaterials within the polymer matrix.19
February, 2015. Prior to his
Nanomaterials have attracted considerable attention in the eld
appointment, he had served at
of material science owing to their excellent physiochemical
the Institute for Nanoscience &
properties, which are not possessed by their micro and macro-
Engineering, University of
scale analogs.20 Several nanomaterials, such as nanostructured
Arkansas and Dental Research
metals and metal oxides (Ag, Au, ZnO, etc.), nanostructured
Institute of Seoul National
carbon in different forms (fullerenes, CNTs, and graphite),
University (SNU) as a post-
nanozeolites, and nanocellulose are frequently used to improve
doctoral fellow aer receiving his
the properties of native (pure) polymers.21–25
PhD in Biosystems & Biomaterials Science and Engineering from
Owing to its large surface area (150–250 m2 g1), high tensile
SNU. His research interests center on improving the understanding,
strength (7.5–7.7 GPa) with Young's moduli of 110–220 GPa,26
design, and performance of biophysical engineering approaches in
excellent optical properties, eco-friendly nature, low density,
molecular & cellular mechanics for controlled stem cells converging
and biodegradability, nanocellulose has recently gained
the bio/nano-technologies.
19144 | RSC Adv., 2019, 9, 19143–19162 This journal is © The Royal Society of Chemistry 2019
Review RSC Advances
Table 1 Comparative study of different types of nanocellulose. Table obtained from ref. 16; published by The AIMS Press
Nanocellulose Typical sources Approximate dimensions Advantages
Cellulose nanocrystals (CNCs) Hardwood, sowood, plants, 4–70 nm in width and 100–6000 nm High surface area, excellent
agricultural residues, bacteria, etc. in length mechanical properties, low density
and low coefficient of thermal
expansion
Cellulose nanobrils (CNFs) Hardwood, sowood, plants, 20–100 nm in width, and Low density, high surface area, and
agricultural residues, bacteria, etc. >10 000 nm in length good mechanical strength
Bacterial nanocellulose (BNC) Low molecular weight sugars such 10–50 nm in width, and >1000 nm Excellent mechanical strength, high
as glucose in length purity, and greater stability
Amorphous nanocellulose (ANC) Cotton, wood pulp 20–120 nm in width, and 50–120 nm High content of functional groups
in length and high sorption ability
Cellulose nanoyarn (CNY) Cellulose and cellulose derivatives 100–1000 nm in width, and High surface area, and high blotting
>10 000 nm in length ability
immense attention in the eld of nanohybrids for the devel- Recently, polymer nanohybrids based on nanocellulose as
opment of bio-based nanomaterials, such as polymer nano- a ller material have drawn signicant attention in the eld of
hybrids, mechanically adaptive materials, and mesoporous materials science and tissue engineering owing to their versatile
photonics solids.27,28 The presence of hydroxyl groups in the nature. Nanohybrids exhibit signicantly superior mechanical
nanocellulose surface provides a platform for chemical func- and optical properties to those of pure polymers.31 Furthermore,
tionalization reactions, such as oxidation, etherication, ester- nanohybrids with nanocellulose as the ller material show
ication, silylation, and polymer graing, enabling the higher biocompatibility than their native polymers.32
nanocellulose to disperse more effectively in various types of Herein, we have described an approach to isolate nano-
polymer matrix materials.29 Thus, nanocellulose can be used as cellulose from different natural sources, its inuence on the
a nanoller.3,30 Fig. 2 shows a few possible methods for the polymer behavior, and its functional applications. The effects of
chemical functionalization of nanocellulose structures.29 the nanocellulose content on the structural, morphological,
Fig. 2 Some common surface modification of nanocellulose: (clockwise from top-right) sulfuric acid treatment provides sulfate esters,
carboxylic acid halides create ester linkages, acid anhydrides create ester linkages, epoxides create ether linkages, isocyanates create urethane
linkages, TEMPO mediated hypochlorite oxidation creates carboxylic acids, halogenated acetic acids create carboxymethyl surfaces, and
chlorosilanes create an oligomeric silylated layer. Reproduced with permission from ref. 29; published by The Royal Society of Chemistry.
RSC Advances Review
mechanical, and optical properties and biocompatibility have and post-production modication. However, the technological
been investigated in detail. Nanocellulose-based nanohybrids production of BNC is still extremely expensive and large efforts
have great potential in biomedical applications such as tissue need to enhance BNC from food to a new generation sophisti-
engineering and wound dressing. Further, the removal of toxic cated materials for different applications such as pourable and
ions from polluted media through nanocellulose-based hybrids spoonable dressings, cultured dairy products, wound care
membranes represent a new, fascinating strategy for water dressing and in burn therapy, etc.45
purication. A schematic representation of the process of extraction of
nanocellulose and other chemicals from raw biomass is shown
2. Extraction of nanocellulose in Fig. 3; this includes the pretreatment of raw materials for the
isolation of cellulose from non-cellulosic materials and further
Several steps including washing and drying, grinding, alkali treatments for specic applications.46 A schematic representa-
treatment, delignication, and acid hydrolysis are involved in tion of the process of CNF and CNC extraction from ber cell
the extraction of nanocellulose from raw biomass. These treat- walls through mechanical and chemical treatments are shown
ments cause the removal of other non-cellulosic components, in Fig. 4.30
such as lignin, hemicellulose, and wax, surrounding the cellu-
lose structure. Furthermore, the acid treatment causes the
dissociation of amorphous zones, leading to the generation of
3. Synthesis of polymer nanohybrids
crystalline CNCs. On the other hand, the mechanical disinte- Nanocellulose is oen used as a ller material to enhance the
gration of cellulosic materials forms a web-like structure with native properties of polymers. Several methods have been used
amorphous and crystalline parts known as CNFs.33 Nano- for the synthesis of polymer nanohybrids; including solution
cellulose can also be obtained through microbial actions in the casting, melt extrusion, and in situ polymerization. In this
form of BNC. It is important to note that chemical constituent section, we describe this these methods, along with their
of all these nanostructured cellulose types are similar but their advantages and disadvantages.
solid-state and physical properties are signicantly different.34
Commercially available microcrystalline cellulose (MCC) and 3.1. Solution casting technique
other non-wood plants, e.g., jute, cotton, leaves, and rice husk,
This is the most common method used for the synthesis of
are also used for nanocellulose extraction.35–38 To obtain the
polymer nanohybrids. In this process, the ller is dispersed in
nanostructured cellulose from cellulose, it is necessary to break
a suitable solvent through sonication or mechanical stirring
down the hierarchical structure of cellulose in at least one
followed by the dissolution of the polymer in the same solvent.
dimension in the nanometer scale.39 This pretreatment requires
Then, the solutions are mixed at or above room temperature.
the removal of the amorphous regions. This includes the
Nanohybrid lms are obtained by either casting the solution or
grinding and an alkali treatment (NaOH 4%, 80 C) of the raw
precipitation.47
material followed by a bleaching process with oxidizing agents
such as NaClO2, in order to remove the lignin and hemicellulose
from the matrix.40 The acid hydrolysis and mechanical disin- 3.2. In situ technique
tegration of the pretreated material lead to the formation of Here, the llers are dispersed in a suitable solvent at the early
CNCs and CNFs, respectively.29,41,42 The properties of the ob- stage of polymerization, and curing agents or chain extenders
tained CNCs are highly inuenced by the hydrolysis duration are added for polymerization at a suitable temperature. This
and the nature and concentration of the acid.3 It is important to technique provides a homogenous dispersion of the ller in the
note that hydrolysis with sulfuric acid is preferred to that with polymer matrix, thereby improving the nanohybrid properties
other acids because it produces charge moiety on the nano- signicantly through stronger interactions.47
structured cellulose, which forms a more stable suspension. In
addition, the steam explosion process (14–16 bar at 200–270 C) 3.3. Melt blending technique
of raw materials for a short time (20 s to 20 min) has also been
Here, an extruder is required to generate high shear forces at
used as a pretreatment, to deconstruct the hierarchical struc-
high temperatures.48 The nanomaterial is incorporated into the
ture of the cellulose. This method is more effective for hard-
molten polymer matrix, which is sheared at a high rate. The
wood cellulosic materials than for sowood ones.40
most signicant advantage of this technique is that no addi-
Nanocellulose can also be obtained from glucose through the
tional solvents are required. However, degradation of the poly-
action of bacteria such as Acetobacter xylinus and Acetobacter
mer chain may occur due to the high temperature and shear
hansenii.43 For this process, bacteria are grown in a medium
forces.49
with proper carbon and nitrogen concentrations for several days
at 30 C.44 The purication of the obtained BNC is carried out by
washing it thoroughly with an alkaline solution and water. The 4. Effects of nanocellulose on
obtained BNC are dimensionally uniform and homogeneous.3 polymer properties
Several efforts have been made for economical production of
BNC through different approach such as fermentation systems, The interactions between the polymer matrix and the functional
genetic engineering, evaluation of culture media compositions, groups in the nanocellulose have a strong inuence on the
Review RSC Advances
Fig. 3Schematic representation of biomass bio-refinery to nanocellulose intermediate and chemicals. Figure obtained from ref. 46; published
by The Hindawi Publisher.
overall properties of the developed nanohybrids. This interac- compatibilizers.50 In the rest of this section we describe the
tion depends mainly on the distribution of the nanocellulose in effects of the nanostructured cellulose on various properties of
the matrix. Weak interfacial interactions between the non-polar the polymer, including the structural, morphological,
polymer matrix and the hydrophilic nanocellulose have been mechanical, thermal, and optical properties by considering
previously reported.30 This drawback is addressed by surface a few common examples. These properties determine the
functionalization of nanocellulose or incorporation of
RSC Advances Review
Fig. 4 Schematic illustration of CNF and CNC production from fiber cell walls by mechanical and chemical treatments, respectively. Reproduced
with permission from ref. 30; Copyright 2014, Elsevier.
potential applications of the developed material and, therefore, cross-linked hydrogels using two different CNF sources with
need to be evaluated for each developed nanohybrid. poly(methyl vinyl ether-co-maleic acid) and polyethylene glycol.
In SEM images of the fractured surfaces of the cross-linked
4.1. Structural and morphological properties of nanohybrids samples, they observed a rougher morphology than in those
The properties of nanohybrids are highly inuenced by the of the non-cross-linked samples. This is because the cross-
nature and dispersion of the ller in the polymer matrix. Khan linked network structure causes the samples to be stretched
et al. reported a CNC-induced trans-crystallization in chitosan more. In addition, non-cross-linked samples showed a relatively
polymers, which led to the improvement of the barrier proper- open structure with a different pore size, much greater than
ties of the nanohybrids.51 However, an increase in the amor- those in the cross-linked samples.57,58 The topographical
phous nature was observed in polymer-graed magnetic behavior of the nanohybrids is also inuenced by the duration
nanocellulose hybrids, which might be responsible for the of the ller incorporation in the polymer matrix process during
enhancement in their hydrophilicity and adsorption capacity.52 polymerization. Boujemaoui et al. reported the morphological
Similar observations were also reported by Anirudhan et al. in differences between two nanohybrids utilizing CNF as the ller
nanocellulose/nanobentonite composites attached with multi- in a poly(methyl methacrylate) (PMMA) matrix. By analyzing
carboxyl functional groups as adsorbents for the removal of SEM images, they observed that graed (mCNF-g-PMMA)
cobalt(II).53 Fig. 5i shows the XRD patterns of PANi- nanohybrids exhibit a more compact layered structure than the
nanocellulose nanohybrids synthesized by in situ oxidative blended (mCNF-b-PMMA) nanohybrids; this is because the CNF
polymerization of aniline on the surface of CNCs. It was network was embedded within the methyl methacrylate (MMA)
observed that the crystalline nature of nanocellulose was sup- monomers prior to polymerization. The SEM images of the cryo-
pressed by the addition of the polymer. Furthermore, the crys- fractured surfaces of the graed and blended nanohybrids are
tallinity of nanohybrids can be enhanced by increasing the shown in Fig. 5ii.59 The in situ polymerization of poly(vinyl
content of CNC in the polymer matrix.54 A comparative study acetate) using vinyl acetate monomers in the presence of CNC
was performed by Abraham et al. to evaluate the effects of yields a more homogenous and ductile fracture surface
nanocellulose in non-cross-linked and cross-linked natural compared to that of physically mixed hybrids.60 A notable
rubber composites. They observed that nanocellulose agglom- improvement in the coating properties was observed in
eration was higher in the latter and inuenced the overall composites synthesized using TEMPO-functionalized CNF with
properties of the developed materials.55 However, no signicant zirconium alkoxide and an epoxy-functionalized silane. The
change in crystallinity was observed in poly(3-hydroxybutyrate) SEM images indicated a decrease in the roughness from
(PHB)-based bionanocomposites synthesized via solution composite coating compared to that of the native materials; the
casting using CNC as a ller material.56 roughness further decreased as the content of CNF in the matrix
The morphological behavior of nanohybrids is highly increased. This is due to the strong interaction between the
affected by the compatibility of the ller with the polymer polar groups in the matrix and the functionalized CNF.61 Zhang
matrix and the interactions between the polymer and the ller et al. studied the inuence of the vinyl monomer concentration
material. Nair et al. successfully prepared cross-linked and non- on the nanocomposites. A rod-like surface morphology with
Review RSC Advances
Fig. 5 (i) XRD-pattern of nanocellulose, pure PANi and PANi/nanocellulose hybrid. Reproduced with permission from ref. 54; published by The
Royal Society of Chemistry, (ii) surface morphology of nanocellulose based PMMA hybrids. (a, d and g) Schematic representation of the relative
CNF/PMMA distribution and SEM images of cryo-fractured surface of (b and c) CNF blended with PMMA (CNF-b-PMMA), (e and f) modified CNF
blended with PMMA (mCNF-b-PMMA), and (h and i) modified CNF grafted with PMMA (mCNF-g-PMMA). Reproduced with permission from ref.
59; Copyright 2018, American Chemical Society, and (iii) 5 mm 5 mm AFM images of (a) 5 (z-scale: 800 nm) and (b) 10 (z-scale: 600 nm) layers of
CNC-PANI ink and (c) 5 and (d) 10 layers (z-scale: 1000 nm) of the PANI ink printed on MLCC paper and (e) the bare MLCC paper substrate (z-
scale: 600 nm). Reproduced with permission from ref. 64; published by The Royal Society of Chemistry.
a core–shell structure was observed in PANi-CNC hybrids when on the interactions between the polymer matrix and the nano-
the aniline monomer concentration was low during the chem- structured cellulose. Better interactions through homogenous
ical oxidative polymerization process on the surface of the dispersion lead to a signicant improvement in the crystallinity
CNC.62 Using atomic force microscopy, Fernandes et al. studied through the nucleating effect of nanostructured cellulose.
the surface topography of chitosan/BNC nanohybrids; they Smoother surface morphologies, attributed to stronger inter-
observed a granular morphology of pure chitosan, whereas the actions, were observed in nanohybrids compared to those of
nanohybrids displayed randomly assembled BNC.63 Fig. 5iii pure polymers. More examples of the applications of
shows the surface morphology of a multilayer curtain-coated nanocellulose-based polymer hybrids in biomedicine and water
(MLCC) paper printed using conducting ink based on polyani- purication will be given in the Applications of nanocellulose-
line and CNC hybrids synthesized by emulsion polymerization based hybrids section.
using a dodecylbenzenesulfonic acid (DBSA). The layers printed
with pure PANi ink exhibit a more dispersed globular micro-
structure with a considerably higher roughness than the layers 4.2. Mechanical properties of nanohybrids
printed with the PANi-CNC ink.64 In this section, we have dis- The mechanical behavior of nanohybrids is signicantly inu-
cussed the effects of nanostructured cellulose on polymers in enced by the volume fraction of the ller and its aspect ratio,
terms of their crystallinity and surface morphology by consid- orientation, and stress transfer, as well as the ller–matrix
ering different examples. It was interesting to note that the interactions. In general, the mechanical behavior of nano-
properties of the developed nanohybrids are highly dependent hybrids has been studied in terms of the content and surface
RSC Advances Review
modication of the llers, and in relation to the coupling nature of the ller, such as the aspect ratio, whereas the tensile
materials used.65 A signicant improvement in the mechanical strength is dependent on the matrix behavior. For CNC/
properties was observed in PEG-graed CNF and poly(L-lactide) carboxymethylcellulose (CMC) hybrids, an improvement in
(PLLA) composite over the native PLLA, due to the reinforce- mechanical responses, including the stiffness and strength, was
ment effect of CNF in the polymer matrix and the inhibition of observed due to efficient stress transfer from the polymer
crack propagation. The mechanical behavior of composite lms matrix to the CNC through strong hydrogen bonding.68 A
with different CNF contents is depicted in Fig. 6i.66 Lee et al. comparative study of the mechanical behavior of nanohybrids
studied the mechanical response of CNC/poly(vinyl alcohol) was performed by Huan et al. to evaluate the reinforcement
(PVOH) hybrids and observed that the CNC enhanced the effect of CNC in electrospun poly(lactic acid) (PLA) brous
crystallinity and alignment of PVOH by acting as a direct rein- hybrids for two different ller orientations (aligned and
forcement, thereby improving the stiffness and strength of the random). They observed a signicant enhancement in the
nanohybrids. A large enhancement in strength (880 MPa) and tensile strength and Young's modulus at a low concentration of
stiffness (29.9) was observed when loading 40 wt% of CNC in the CNC (10 wt%), and a deterioration of the same properties at
polymer matrix.67 The Young's modulus is highly affected by the higher concentrations; this is attributed to more efficient stress
Fig. 6 (i) Mechanical properties of nanocomposite films with different cellulose nanofibril contents: (a) stress–strain curves, (b) Young's moduli,
(c) ultimate tensile strengths, and (d) work of fractures. Reproduced with permission from ref. 66; Copyright 2013, American Chemical Society,
and (ii) typical oscillatory rheological behavior, as shown by the nanohybrid hydrogel with a 1.5 wt% cellulose nanocrystal (CNC) and 1.0 wt%
methyl cellulose (MC) loading: (a) frequency sweep preformed between 0.1–300 rad s1 at 60 C (red) and 20 C (blue), determined at 10% strain;
(b) strain sweeps at 60 C (red) and 20 C (blue), determined at an angular frequency of 6.283 rad s1. The linear low strain G0 value was ca. 510 Pa
at 60 C. Reproduced with permission from ref. 75; Copyright 2014, American Chemical Society.
Review RSC Advances
transfer from the PLA to the stiffer (at a lower concentrations) achieved at 60 C. Their obtained values of the storage modulus
nanocellulose;69 on the other hand, at higher concentrations, (G0 ) were higher than those of the loss modulus (G00 ) due to the
the CNC agglomerate, resulting in a decrease in the crystallinity. physical cross-links between the methylcellulose and CNC.75
This behavior is similar for both random and aligned ller These examples clearly indicate that the mechanical properties
orientations; however, in all cases, the improvement in the of nanohybrids are highly inuenced by the nature and content
mechanical properties was much better with the aligned ller of the ller, and the interactions between the nanostructured
compared to the randomly oriented one.70 The incorporation of cellulose and the polymer matrix. These results indicate that
5% (w/w) CNC in the chitosan matrix resulted in a 26% increase nanostructured cellulose can act as a reinforcing agent at a low
in the mechanical properties, compared to the native polymer.51 concentration in solid and at melt conditions.
Starch/CNF-based foam nanohybrids at lower concentrations of
CNF (40 wt%) also exhibited an improvement in the mechanical 4.3. Thermal properties of nanohybrids
properties, which deteriorated with increasing CNF content.
The physical and mechanical responses of CNF-based foam The thermal stability is another important parameter for hybrid
composites with varying contents of CNF are listed in Table 2.71 materials; it indicates the temperature range at which materials
In another study, it was observed that the addition of 4% lignin- are stable and is measured by thermogravimetric analysis
coated CNC in an acrylonitrile butadiene styrene (ABS) matrix (TGA). The dispersion of the ller material in a polymer matrix,
resulted in an increase in the tensile and storage moduli. surface functionalization or adhesion of the ller, and thermal
Furthermore, a deterioration in mechanical properties was stabilities are the important criteria for the development of
observed at a higher content of the ller, due to the poor reinforced hybrids.65 Razalli et al. synthesized polyaniline/CNC
interfacial interaction between the polymer and CNC.72 The hybrids through the in situ oxidative polymerization of aniline
mechanical strength of the hybrid under melt/liquid conditions in the presence of CNC isolated from Semantan bamboo and
is governed by several important factors, such as the distribu- observed an improvement in the thermal stability of the nano-
tion and dispersion of the ller and its compatibility with the hybrids compared to that for pure PANi and CNC, indicating
polymer matrix and interfacial interactions. Castro et al. studied a greater interaction between the matrix and CNC and the
the mechanical response of poly(vinyl alcohol) (PVA)/BNC protection of the PANi layered by the CNC.54 Similar types of
hybrids synthesized in situ and noted that nanohybrids have degradation behaviors were also observed by Casado et al. in
a higher storage modulus (G0 ) than their native polymers. This PANi/CNF hybrids.76 In another study, Gwon et al. synthesized
was attributed to the reinforcement effect of BNC via hydrogen poly(lactic acid) (PLA)-based CNC composites using two
bonding with the polymer matrix, which is also responsible for different CNC, namely pure CNCs and toluene diisocyanate-
the improved mechanical response of the nanohybrids. The modied CNC, and evaluated their thermal stabilities by TGA
reinforcing effect of nanomaterials is highly dependent upon measurements. They observed that the composites made by
the effective stress transfer between the polymer matrix and the modied CNC exhibited lower thermal stability than pure PLA
ller material.73 Ago et al. investigated the effect of CNC on the and the PLA/CNC composite. This is due to the homogenous
mechanical properties of lignin-PVA/CNC-based composite dispersion of the functionalized CNC in the polymer matrix,
under melt conditions. They observed that as the content of which enhanced the heat transfer rate in the PLA lm, leading
CNC increased with a xed ratio of the lignin-PVA matrix, the to faster degradation.77 However, an enhancement of thermal
storage modulus (G0 ) increased. This is due to the presence of stability in the presence of CNC in the PLA matrix was reported
a strong interconnected network structure in the nanohybrids.74 by Lu et al., who noted that the thermal stability is highly
McKee et al. studied the inuence of CNC on the mechanical dependent upon the functionalization and preparation proce-
properties of thermoresponsive methylcellulose (MC) hydrogels dure of the CNC.78,79 Fig. 7i and ii presents a thermogram of
under melt conditions, as shown in Fig. 6ii. They noted that by PLA/CNC hybrids and indicates that a signicant improvement
increasing the content of CNC from 0 to 3.5 wt%, the storage in the thermal stability was obtained in nanohybrids due to the
modulus was enhanced; in contrast, a distinct gel state was more efficient dispersion of the ller and the stronger interac-
tions between the ller and polymer matrix. Thermal analysis
Table 2 Physical and mechanical properties of MFC reinforced amylopectin-based foam with varying MFC contents. The samples have been
conditioned in 50% relative humidity and 22 C for 48 h. The values within parenthesis are the sample standard deviation. Reproduced with
permission from ref. 71; Copyright 2008, Wiley Publication
Young's Yield strength Water content

MFC (wt%) modulus (MPa) (kPa) Density r* (kg m3) Relative density, (r*/rs)a (%)
0 4.9 (1.1) 170 (25) 103 (2.08) 0.084 11.0

10 5.0 (1.0) 310 (91) 109 (2.79) 0.088 10.3
40 7.0 (0.61) 510 (21) 95.1 (1.02) 0.073 8.4
70 1.7 (0.40) 110 (78) 86.5 (1.29) 0.063 7.3
a
The theoretical density of the cell wall.
RSC Advances Review
Fig. 7 (i) TGA, and (ii) DTA curve of PLA and its indicated nanohybrids. Reproduced with permission from ref. 80; published by The Royal Society
of Chemistry.
results for pure PLA and its nanohybrids at different ller a decrease in the glass transition temperature (Tg) and melting
contents are given in Table 3.80 Incorporation of BNC into temperature (Tm) was observed in chitosan/nanocellulose
a poly(vinyl alcohol) (PVA) matrix led to an interesting hybrids in the presence of glycerol. This decrease was due to
improvement in the thermal stability at higher temperatures an increase in the movement of the chitosan chains and
compared to that of pure PVA, possibly due to the better a decrease in the crystallinity.83 Mandal et al. synthesized linear
dispersion and excellent compatibility between the PVA matrix and cross-linked PVA-based hybrids using bagasse-extracted
and the BNC.73 This is further supported by differential scan- nanocellulose and evaluated their thermal behavior. They
ning calorimetry (DSC) measurements, where an improvement noted that nanohybrids exhibited higher thermal resistance
in the glass transition temperature (Tg) and melting tempera- than pure PVA and cross-linked hybrids. This is due to the
ture (Tm) was observed in nanohybrids. This can be attributed to interlocking of hydroxyl groups of PVA via hydrogen bonding
the strong interaction and excellent compatibility between the and the formation of a cross-linked network structure, which
matrix and ller, causing a decrease in the mobility of the PVA requires a much higher energy to break.84 These results high-
chains at the interface.81 The thermal transition and BNC- lighted that the thermal stabilities of hybrids are highly affected
induced melting behavior measurements of nanohybrids at by the compatibility of nanostructured cellulose with the poly-
various ller concentrations are shown in Table 4.73 An mer matrix. The higher compatibility of nanostructured cellu-
improvement in the thermal properties of nanohybrids was also lose with the matrix facilitates the improvement in the thermal
reported by Cho et al. in poly(vinyl alcohol)/CNC hybrids behaviors of hybrids through stronger interactions. Thermal
synthesized using commercial MCC via a casting technique. At properties such as the melting, glass transition, and crystalline
lower contents of nanocellulose (1 wt% and 3 wt%), no signif- temperatures are not directly related to the biomedical appli-
icant improvement in the thermal stability was observed. cations of hybrid materials but provide important information
However, at a higher content of CNC (5 wt%), the nanohybrids on the best processing conditions for biomedical polymers into
exhibited higher thermal stability.82 Moreover, in another study, implants or devices. In addition, the thermal stability of mate-
rial provides information on their applications range. More heat
Table 3 Thermal analysis parameters for pure PLA, SCNFs and the
nanohybrids with various SCNF (spherical nanocellulose formats)
content. Reproduced with permission from ref. 80; published by The Table 4 Thermal transitions and crystallinity (a) of matrices and cross-
Royal Society of Chemistrya linked nanohybrids reinforced at various BC loadings. Reproduced
with permission from ref. 73; published by The Royal Society of
Samples Tob ( C) T5%b ( C) Tmaxb ( C) Tfb ( C) Ea (kJ mol1) Chemistry
PLA 335.7 325.9 354.6 363.9 319.95 DH

1 wt% 336.3 327.0 357.0 369.4 360.13 Samples Tg ( C) Tm ( C) (J g1) Xc (%) Xp (%)
3 wt% 342.2 332.4 361.6 371.5 380.61
5 wt% 342.6 333.0 363.1 372.3 407.57 PVA 10 76.2 224.7 69.7 0.43 0.43
10 wt% 353.8 342.2 376.1 390.0 414.77 PVA/BC 10(10) 79.7 236.4 68.3 0.42 0.47
15 wt% 350.8 338.9 373.5 383.4 395.16 PVA 5 69.2 225.3 73.3 0.45 0.45
20 wt% 346.6 331.4 366.3 379.2 373.37 PVA/BC 20(5) 78.8 230.6 48.1 0.30 0.37
SCNFs 323.1 292.2 358.0 368.3 248.3 PVA 2.5 63.5 228.1 59.3 0.37 0.37
a
PVA/BC 30(2.5) 84.2 229.8 43.9 0.23 0.33
Ea (activation energy). b To, T5%, Tmax, and Tf were obtained from the
TGA curve at a heating rate of 10 C min1. a
Xc ¼ DHm/DH0m and Xp ¼ Xc/w; with DH0m ¼ 161.6 J g1.
Review RSC Advances
resistant and longer-term thermal properties make polymeric 5. Applications of nanocellulose-

membranes suitable candidates for water treatment.
based hybrids
5.1. Tissue engineering applications
Nanocellulose and its hybrids are frequently used for fabri-
4.4. Optical properties of nanohybrids cating a variety of devices, such as medical implants, drug
delivery vectors, and vascular gras; moreover, owing to their
The optical transparency is a critical parameter for building sustainability, biodegradability, and biosafety they are used for
light-transmitting materials and solar cell windows and tissue engineering applications.120–123 In addition, high water-
ophthalmic devices. For these applications, materials should be holding capacity with better elasticity and conformability and
highly transparent. Multifunctional lightweight, transparent, excellent mechanical strength make nanocellulose an ideal
and mechanically strong polymer-based composites are highly material in wound-care dressing applications.124 It has been
desirable for several applications. Geng et al. synthesized highly noticed that CNC have antimicrobial activity, which provides an
ordered, transparent, and mechanically strong nanohybrids additional advantage for wound-dressing applications.125
using CNF in a PLA matrix. They observed that chemical gra- Notably, more efficient cell adhesion, proliferation, and
ing of CNF with the PLA matrix resulted in a more aligned and migration were observed in CNC environments. This is due to
transparent material than physically blended nanohybrids.85–87 the high aspect ratio and good biocompatibility of CNC, which
The inuence of the solvent ratio and the type of nanocellulose facilitate cellular activities.6
(CNCs and CNFs) on the optical transparency of poly(vinyl Here, we give a few examples of nanocellulose-based polymer
alcohol) hydrogel, was studied by Tummala et al. They observed hybrids and describe their tissue engineering applications. In
a decrease in the optical transparency of CNFs in the visible these examples, a signicant change in cellular responses was
range due to the agglomeration of the polymer chains in the observed in the presence of nanocellulose-based hybrids at low
media with more aqueous conditions.88 On the other hand, concentration, indicating their potential as biomaterials for
nanohybrids having CNCs in their polymer matrix showed tissue engineering. The cytotoxic behavior of maleic acid (MA)-
a more transparent nature in the visible range than the CNF- graed poly(butylene adipate-co-terephthalate) (MA-g-PBAT)
based hybrids. This is due to the smaller aspect ratio and hybrids on L929 broblasts in the presence of different
lesser light-scattering tendency of the CNC compared to CNFs. concentrations of CNCs at different time intervals was studied
Fig. 8i presents the UV-visible transmittance spectrum of PVA by Rahimi S K et al. using an MTT assay. No notable cytotoxic
hydrogel for different solvent ratios and nanocellulose effects were observed aer 72 h of incubation, indicating the
concentrations.31 Lightweight, optically transparent, and biocompatible nature of the developed material. Fig. 9i presents
mechanically enhanced wood was synthesized by pre- a cell viability test by MTT assay at different time intervals and
polymerized MMA and a de-lignied porous wood concentrations of CNC in the hybrids.126 In addition, many
template.89,90 The optical properties of the synthesized wood can studies have been conducted on various nanocellulose-based
be altered by changing the cellulose content.91 The optical polymer hybrids, such as collagen,127 poly(lactic acid),128 and
transparency of materials can be tuned using suitable plasti- polyurethanes,129 to evaluate their cytotoxic effects on different
cizers.92,93 The effect of the ionic crystal, 1-allyl-3- cells in a culture media. The effect of CNC on the behavior of
methylimidazolium chloride (Amim Cl), on the optical trans- a poly(vinyl acetate) (PVAc)-coated poly(lactic acid) (PLA) lm in
parency of CNC was studied by Liu et al., who observed that with the presence of NIH-3T3 mouse broblasts was studied by
an increase in the ionic liquid content during the ltration Hossain et al. They observed that the surface of the nanohybrids
process, the color changed from light brown to light blue due to was completely covered by the broblasts, due to their contin-
the strong interactions between the polar groups of the CNC uous proliferation and spreading, forming a multilayered
and the ionic liquid.94 In another study, a decrease in the optical cellular structure aer 24 h of incubation; only a few rounded
transmittance of chitosan/CNF composite was observed when cells were observed.114 The effects of the type of material and
the content of TEMPO-modied CNF in the polymer matrix was surface roughness on the morphology and spreading of NIH-
increased.95 The inuence of the CNF on the optical trans- 3T3 cells at different time intervals are shown in Fig. 9ii. In
mittance of uniform and exible magnetic nanopapers another study, Tang J. et al. synthesized poly(vinyl alcohol)
synthesized by immobilization of Fe3O4 nanoparticles was (PVA)-doped BNC tubular hybrids through a thermally induced
studied by Li et al. They noted that the fabricated nanopapers phase separation method for articial blood vessel-based
are transparent in the visible range with excellent exibility, and applications. The cytotoxic behavior of the developed hybrids
that the transparency of the developed magnetic papers can be towards pig iliac endothelial cells (PIECs) at different time
tuned by changing the content of Fe3O4 nanoparticles.96 A intervals was monitored using an MTT assay. It was noted that
digital image of magnetic papers prepared by using CNF and no signicant cytotoxic signature was caused by the nano-
Fe3O4 nanoparticles is shown in Fig. 8ii. The transparency of hybrids, and the hybrid tubes enabled a higher proliferation of
these papers can also be improved by reducing their thickness, the cells, indicating their biocompatible nature.130 Naseri et al.
which will decrease their optical scattering.97,98 Effects of synthesized CNC/sodium alginate and gelatin (SA/G)-based
nanocellulose on the polymer properties are also given in Table hybrids through a freeze-drying process and evaluated their
5.
RSC Advances Review
Fig. 8 (i) Comparative UV-vis transmission spectrum of 1 mm hydrogels with (a) 10% PVA, (b) 10% PVA and 1% CNF, (c) 10% PVA and 1% CNC, and
(d) 10% PVA and 1% CNF/CNC. Reproduced with permission from ref. 31; Copyright 2016, American Chemical Society, and (ii) (a) a digital image of
magnetic paper with 10 wt% Fe3O4 NPs shows the transparency and flexibility, (b) nanopapers with 0 wt%, 5 wt%, and 10 wt% Fe3O4 NP loading
from left to right and (c) transmittance curves of magnetic papers. Reproduced with permission from ref. 96; published by The Royal Society of
Chemistry.
cytocompatibility using mesenchymal stem cells (MSCs). No nature using normal mouse embryonic broblasts. No cytotoxic
sign of cytotoxicity was observed, and the highly porous nature effects of the composites were observed; furthermore, the
of the scaffold of these hybrids was observed to facilitate cell composites with 3% nanocellulose showed a higher level of
proliferation.131 Poonguzhali et al. fabricated chitosan/ antibacterial activity than the hybrids with other nanocellulose
poly(vinyl pyrrolidone)/nanocellulose (CPN) hybrids through concentrations.132 A wound-healing ability with no inamma-
a solution casting technique and evaluated their biocompatible tion effects was also observed for nanohybrids developed by the
Review RSC Advances
Table 5 Effects of nanocellulose on the polymer properties
Polymer matrix Nanocellulose Preparation technique Properties References
Polystyrene (PS) CNC Electrospinning Improvement in tensile 99–101

strength, wettability,
crystallinity, and thermal
decomposition
CNC Extrusion Enhancement in the
mechanical properties,
degradation temperature
CNF-TEMPO Solution casting Enhancement in the
mechanical, thermal, and
optical
Ethylene vinyl alcohol CNC Electrospinning Enhancement in thermal 102 and 103
(EVOH) BNC properties
Poly vinyl chloride (PVC) CNC Hot mixing Enhancement in the 104–106
CNC Solution casting mechanical strength
Polymethyl CNC Solution casting Improvement in the 107–109
methacrylate(PMMA) mechanical and degradation
temperature
CNF Immersion precipitation Enhancement in thermal
stability and storage
modulus
CNF-TEMPO Solution casting Improvement in the
mechanical strength
CNF Solvent exchange Enhancement in 59
mechanical, thermal, and
water content
Polypropylene (PP) CNF Emulsion process Enhancement in the 110 and 111
mechanical strength
CNC Melt extrusion Improvement in the
mechanical, thermal and
crystallinity
Poly(lactide) (PLA) CNC Solution casting Enhancement in thermal, 112 and 113
CNF mechanical and crystallinity
CNF-TEMPO Homogenous dispersion in 66
organic solvents,
improvement in mechanical
strength, and decrease in the
glass transition temperature
CNF Suspension coating Enhancement in the 80
mechanical, thermal and
crystallization behavior
CNC Enhancement in the 114
mechanical, water uptake
and biocompatibility
Polyethylene (PE) CNC Melt extrusion Improvement in thermal 115
and mechanical strength
Polyimide (PI) CNC Spin coating Improvement in thermal, 116
mechanical, barrier and
optical properties
Poly(vinyl alcohol) (PVA) CNC Solution casting Improvement in optical 31
CNF transparency, water content,
BNC In situ polymerization Enhancement in thermal, 73
mechanical, and cell
proliferation
Polyaniline (PANi) CNC In situ polymerization Enhancement in 54
electrochemical properties,
thermal behavior, and
crystallinity
CNC Emulsion polymerization Enhancement in 64
electrochemical properties,
Methylcellulose (MC) CNC Solution casting Enhancement in the 75
mechanical strength
RSC Advances Review
Table 5 (Contd. )
Polymer matrix Nanocellulose Preparation technique Properties References
Poly(butylene adipate-co- CNC Melt extrusion Enhancement in thermal, 117

terephthalate) (PBAT) mechanical, and
biocompatibility
Chitosan CNF Solution casting Enhancement in 118
mechanical, crystallinity and
sustained drug delivery
Poly(N-methacryloyl glycine) BNC In situ polymerization Improvement in 119
biocompatibility and
sustained drug release
in situ preparation of silver nanoparticles embedded within external electric elds. These examples demonstrated a very
a bamboo nanocellulose matrix.133 controlled release of the loaded drugs in different conditions
and show their potential use as carriers in drug delivery appli-
5.2. Drug delivery cations. The effect of the nanocellulose on the ketorolac tro-
methamine (KT) drug-delivery behavior of chitosan was studied
One of the critical issues of using polymeric materials as
by Sarkar et al. Drug-loaded samples were synthesized by solu-
implants is that the polymer should release the biologically
tion casting. The nanohybrids exhibited more sustained drug
active bound material at a suitable rate and for the required
release compared to the pure chitosan; this behavior was more
period of time, which are dependent on the biological condi-
sustained in nanohybrids with a higher content of nano-
tions.134,135 Controlled drug release is a very important factor to
cellulose. This is due to the greater interaction between the
maintain the drug concentration within the therapeutic window
polymer matrix and ller material, which hinders the diffusion
and achieve the minimum side effects and maximum thera-
pathways and reduces the drug uptake and release.138,139 Fig. 10i
peutic effects of the drug.136 Several factors, such as the inter-
presents an in vitro drug release prole of the pure polymer and
action between the drug and the polymer matrix, the solubility
its nanohybrids.118 Shi et al. synthesized the BNC/sodium algi-
of the drug, and the swelling tendency of lms in different
nate hybrid hydrogels for controlled drug delivery induced by
media play an important role in the release of drugs from the
pH and electric stimuli. As the pH of the medium changed from
matrix.137 Here, we describe some examples of nanocellulose-
an acidic to an alkaline value, a faster drug release was observed
based hybrid materials for drug delivery application under
due to the increase in the swelling behavior of the hydrogel in
different conditions, i.e., the content of nanocellulose, pH, and
Fig. 9 (i) MTT assay cell viability of L929 cells for (a) MA-g-PBAT, (b) CNC, (c) 3% CNC, and (d) 9% CNC samples at specified incubation times.
Reproduced with permission from ref. 126; Copyright 2017, American Chemical Society, and (ii) influence of materials and surface roughness on
NIH-3T3 mouse fibroblast cell morphology and spreading at varying time points (4, 24, and 48 h): (a) control PLA, (b) PLA CNW-75, (c) PLA PVAc,
and (d) control TCP (tissue culture plastic). Reproduced with permission from ref. 114; Copyright 2014, American Chemical Society.
Review RSC Advances
Fig. 10 (i) Drug release profiles of polymer and it's indicated nanohybrids. Reproduced with permission from ref. 118; published by The Royal
Society of Chemistry, and (ii) diclofenac dissolution profile at pH 2.1 (,) and 7.4 (B) from PMGly/BC/DCF nanocomposite membrane. The lines
are for visual guidance only. Reproduced with permission from ref. 119; Copyright 2017, Elsevier.
the alkaline medium, causing an easier diffusion of the drug. 5.3. Water purication
Moreover, by changing the electric eld from 0 to 0.5 V, the drug With increasing populations and industrialization, the removal
release from the hybrid hydrogels becomes faster. This is of heavy metal ions has become a challenging task for human
attributed to the swelling nature of the hybrid hydrogels.140
society today. Conventional methods such as ltration, chem-
Non-cytotoxic and pH-sensitive hybrids were synthesized by
ical precipitation, electrochemical treatment, ion exchange,
Saidi et al. using poly(N-methacryloyl glycine) and nano-
membrane technologies, evaporation and adsorption of acti-
cellulose under green-reaction conditions. They observed that
vated carbon, etc., are used for removal of toxic ions from
faster drug release occurred at a higher pH (7.4) than at a lower
wastewater. However, these methods have some disadvantages
pH (2.1). This is due to both the pH-dependent solubility of the
such as limited range, expensive technology, and energy
loaded drug (diclofenac sodium salt, DCF), which has poor intensive.156 These limitations can be overcome by biosorption
solubility in acidic environments,141 and the pH sensitivity of which has the potential to remove the metal ions in solution
the nanohybrids due to the presence of amino acid properties,
from ppm (parts per million) to ppb (parts per billion)
which show poorer water–uptake properties under acidic
level.157–159
conditions.119 An in vitro drug release prole of the composites
Cellulose-based adsorbent materials have drawn signicant
under different conditions is shown in Fig. 10ii. Nanocellulose-
attention due to their hydrophilicity, and functionalization
based polymer nanohybrids for tissue engineering applications
ability, and easy to tune the different properties such as surface
are also summarized in Table 6.
area, aspect ratio, as well as chemical accessibility.160 However,
conventional cellulose-based adsorbent has limited selectivity
Table 6 Nanocellulose-based polymer hybrids for tissue engineering applications
Nanocellulose-based polymer nanohybrids Nature of materials Applications References
BNC/heparin Scaffolds Tissue engineering 142–149

BNC/potato Starch (PS)
BNC/poly(3-hydroxyoctanoate) (PHO)
BNC/polyvinyl alcohol
BNC/collagen
BNC/silk broin
BNC/Chitosan
BNC/collagen
Poly(oligoethylene glycol methacrylate)/CNCs Injectable hydrogel Tissue engineering 150
CNFs/gelatin Cryogels hydrogels Controlled drug delivery 151–155
CNFs-Ag/alginate Antibacterial
BNC/acrylic acid Drug delivery
BNC/gelatin
CNCs/chitosan
RSC Advances Review
Table 7 Nanocellulose-based materials for application of wastewater treatment
Adsorption potential
Materials Removal of (mg g1) References
Calcium hydroxyapatite/microbrillated cellulose (MFC) Cr(VI) 114.7 170

Aminopropyltriethoxysilane modied (APS)/MFC Ni(II) 159.8 171
Cu(II) 200.1
Cd(II) 471.5
Nanocellulose/nanobentonite composite Co(II) 350.8 172
U(VI) 121.0
Cellulose nanobers (CNF) with positively charged quaternary ammonium groups NO3 44.0 173
F 10.6
SO42 50.0
PO43 55.0
Cationic CNF aerogel with trimethylammonium chloride Blue dye CR 19 230.0 174
Red dye 180 160.0
Orange dye 142 230.0
Amino-modied nanocrystalline cellulose (ANCC) Acid red GR, 134.7 175
Congo red 4BS 199.5
Light yellow K-4G 183.0
Carboxylate-modied cellulose nanocrystal (CNCs) Crystal violet 243.9 176
Methylene blue
Malachite green
Basic fuchsin
CNCs/alginate hydrogel beads Methylene blue 255.5 177
Phosphorylated nanocellulose Ag(I) 100% 178
Cu(II)
Fe(III)
and lower adsorption kinetics due to the limited active sites or 2B, Methyl Violet 2B, and Rhodamine 6G, respectively, aer
surface area and difficult to recover from wastewater. In a contact time of 24 h. This activity of the fabricated membranes
contrast to micrometer-sized cellulose, the nanometer-sized was attributed to the electrostatic interactions between the
cellulose has a larger surface area with improved porosity, positively charged dyes and negatively charged CNC.166 Fig. 10
which provides a great advantage for metal ion removal from presents a naked-eye visualization of the removal efficiency of
wastewater. This improvement in the adsorbent potential of cross-linked hybrid membranes. A thin-lm nanocomposite
nanocellulose is due to the presence of functional groups, (TFN) membrane was synthesized through the in situ interfacial
increased surface area, and crystalline nature.161 In addition, polymerization of MPD and trimesoyl chloride (TMC) by
nanocellulose is thermodynamically stable as compared to incorporating CNCs into the active polyamide layer for water
metallic nanoparticles, which make them a suitable material for desalination. A salt rejection of 97.8% was observed when 0.1%
this application.162–164 The processing of nanocellulose-based (w/v) of nanocellulose was loaded into the matrix, indicating the
membranes for optimal access to functional sites, with high potential for the large-scale use of these nanohybrid
ux and mechanical stability, is a challenging task in water membranes in water desalination.167 Tato et al. synthesized
purication. In generals, lling of electrospun mats with thin-lm composite (TFC) membranes using amino-modied
nanocellulose; vacuum ltration and coating; and freeze-drying nanocellulose with silver and platinum nanoparticles. The
are the most relevant and used techniques for the processing of fabricated thin lms showed nger-like pore morphologies and
nanocellulose-based membranes.165 varying pore sizes, and a high solute rejection of wastewater
Surface hydroxyl groups play an important role in the samples, which indicates their potential as novel water puri-
binding and removal of foreign substances from aqueous cation materials.168 In another study, fully bio-based TFCs were
medium. Here, we describe the water purication capacity of synthesized using cellulose microbers as a support layer and
nanocellulose-based membranes through a few examples. The different CNC concentrations in a gelatin matrix as the func-
selected examples demonstrate the very high water purication tional layer. When treated with mirror industry effluents con-
efficiency (98%) of nanocellulose at a very low content in taining metal ions (Ag+, Cu2+, and Fe2+/Fe3+), the fabricated lm
polymer matrices. The higher dye and metal ion-removal effi- showed a high ion-removal capacity (100% in some cases) and
ciency of nanohybrids, make them suitable membrane mate- a very high water permeability (900–4000 L h1 m2) at pressure
rials for water purication. Karim et al. prepared bio-based below 1.5 bars. The high ion-removal capacity of these
hybrid membranes of chitosan/CNC through freeze-drying, membranes is due to the high level of interactions between
followed by a compacting process for the removal of dyes positively charged metal ions and the negatively charged
from water. These fabricated membranes successfully removed CNCs.169 The nanocellulose-based polymer hybrids used in
98%, 84%, and 70% of the positively charged dyes Victoria Blue water purication are also given in Table 7.
Review RSC Advances
6. Conclusions and future 2018R1A6A1A03025582) and the National Research Foundation

of Korea (NRF-2016R1D1 A3B03932921). The authors also
perspectives acknowledge the Cooperative Research Program for Agriculture
Nanocellulose has drawn a lot of attention from the scientic Science and Technology Development (no. PJ012854012017),
community in recent year, especially in the form of bacterial Rural Development Administration.
cellulose, cellulose nanobrils, and cellulose nanocrystals,
owing to their unique inheritance properties, easy fabrication,
and biodegradability and biocompatibility. Nanocellulose can References
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Nanocellulose-based polymer hybrids and their

Nanocellulose Typical sources Approximate dimensions Advantages

Young's Yield strength Water content

0 4.9 (1.1) 170 (25) 103 (2.08) 0.084 11.0

PLA 335.7 325.9 354.6 363.9 319.95 DH

resistant and longer-term thermal properties make polymeric 5. Applications of nanocellulose-

Table 5 Eﬀects of nanocellulose on the polymer properties

Polymer matrix Nanocellulose Preparation technique Properties References

Polystyrene (PS) CNC Electrospinning Improvement in tensile 99–101

Polymer matrix Nanocellulose Preparation technique Properties References

Poly(butylene adipate-co- CNC Melt extrusion Enhancement in thermal, 117

Table 6 Nanocellulose-based polymer hybrids for tissue engineering applications

Nanocellulose-based polymer nanohybrids Nature of materials Applications References

BNC/heparin Scaﬀolds Tissue engineering 142–149

Table 7 Nanocellulose-based materials for application of wastewater treatment

Calcium hydroxyapatite/microbrillated cellulose (MFC) Cr(VI) 114.7 170

6. Conclusions and future 2018R1A6A1A03025582) and the National Research Foundation

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