![Hierarchical structure of cellulose [8] [Reused with permission from the publisher].](https://www.researchgate.net/publication/371180727/figure/fig1/AS:11431281164083236@1685621438578/Hierarchical-structure-of-cellulose-8-Reused-with-permission-from-the-publisher_Q320.jpg)
![Equipment used for homogenization process; (a) homogenizer (b) microfluidizer [Reused with permission from publisher].](https://www.researchgate.net/publication/371180727/figure/fig3/AS:11431281164053144@1685621439318/Equipment-used-for-homogenization-process-a-homogenizer-b-microfluidizer-Reused_Q320.jpg)
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Review
Harnessing Nature's Ingenuity: A Comprehensive
Exploration of Nanocellulose from Production to
Cutting-Edge Applications in Engineering and
Sciences
A. G. N. Sofiah 1*, J. Pasupuleti 1*, M. Samykano 2, K. Kadirgama 2, S. P. Koh 1, S. K. Tiong 1, A. K.
Pandey 3, 4 and S. K. Natarajan 5
1Institute of Sustainable Energy, Universiti Tenaga Nasional (The Energy University), Jalan Ikram-Uniten,
Kajang 43000, Selangor, Malaysia.
2Centre for Research in Advanced Fluid and Processes, Universiti Malaysia Pahang, 26300 Gambang, Pahang,
Malaysia.
3Research Centre for Nano-Materials and Energy Technology (RCNMET), School of Science and Technology,
Sunway University, No. 5, Jalan Universiti, Bandar Sunway, Petaling Jaya, 47500 Selangor Darul Ehsan,
Malaysia.
4Center for Transdiciplinary Research (CFTR), Saveetha University, Chennai, India
5Solar Energy Laboratory, Department of Mechanical Engineering, National Institute of Technology
Puducherry, Karaikal, UT of Puducherry, India
* Correspondence: jagadeesh@uniten.edu.my (J. Pasupuleti); nurhanis.sofiah@uniten.edu.my (A. G. N.
Sofiah).
Abstract: Primary materials supply is the heart for engineering and sciences; depletion of natural
resources and an increase in the human population by a billion in 13 to 15 years pose a critical
concern on the sustainability of the materials. Therefore, functionalizing renewable materials, such
as nanocellulose, possibly exploiting its properties for various practical applications, has been
undertaken worldwide. Nanocellulose has emerged as a dominant green natural material with
attractive and tailorable physicochemical properties, renewable, sustainable, biocompatibility, and
tunable surface properties. Nanocellulose is derived from cellulose, the most abundant polymer in
nature with remarkable properties of nanomaterials. This article provides a comprehensive
overview of the methods used for nanocellulose preparation, structure-property and processing-
property correlations, and the application of nanocellulose and its nanocomposite materials. This
article differentiates the classification of nanocellulose, provides a brief account of the production
methods that have been developed for isolating nanocellulose, highlights a range of unique
properties of nanocellulose that have been extracted from different kinds of experiments and
studies; and elaborates on nanocellulose potential applications in various areas. The present review
is anticipated to provide the readers regarding the progress and knowledge related to nanocellulose.
Pushing the boundaries of nanocellulose further into cutting edge applications will be of particular
interest for the future, especially as cost-effective commercial sources of nanocellulose continue to
emerge.
Keywords: Nanocellulose; Cellulose Nanofibrils; Cellulose Nanocrystals; Bacterial Nanocellulose;
Energy Storage
1. Introduction
Materials play a dominant role in human life and civilization. Every technological advancement
has been achieved through the discovery of higher-performing materials than its predecessor. Steel,
cement, and polymers are few materials that dominate the structural, construction, and architectural
application domains, whereas silicon dominates the electronics and communication industry [1].
Disclaimer/Publisher’s Note: The statements, opinions, and data contained in all publications are solely those of the individual author(s) and
contributor(s) and not of MDPI and/or the editor(s). MDPI and/or the editor(s) disclaim responsibility for any injury to people or property resulting
from any ideas, methods, instructions, or products referred to in the content.
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© 2023 by the author(s). Distributed under a Creative Commons CC BY license.
Most of the present-day products, including those mentioned above, are built using earth-borne or
non-renewable materials, i.e., their constant stock on the planet would be exhausted as we consume
it. At present, a great deal of research is dedicated to recuperating the earth-born materials (mainly
metals and other inorganic components) from the products after their service life [2]. Adding on,
carbon, a functional material of high market value, is traditionally obtained from petroleum coke,
pitch and coal – which are earth-born and have been extensively researched for potential developed
from renewable sources such as biomass. The above is a partial story of primary material supply for
product development; the other part is the growing population-nearly a billion new members are
expected to join the society in 13-15 years. Thus, a growing population and depleting natural material
reserves demand strategic solutions for primary material supply to build our next-generation
architects and devices. Besides, “renewability” has been evolved as a key term in almost every sector
of life. One unique possibility in searching for a renewable material of diverse functionality is
cellulose, derived from plants and plant-derived wastes. For example, cellulose can be derived from
an empty fruit bunch of oil palm or coconut, which does not offer edibility or other functionality.
Cellulose is the main component of several natural fibers such as cotton, flax, hemp, jute, sisal, etc.
Recently, cellulose has been explored for its applications in electronic devices [3, 4], material sciences
[5, 6], construction[7], and biomedical sciences [8]. The utilization of this particular element can be
traced back to the commencement of civilization, characterized by wood, hay, papyrus, and cotton
as examples of its natural form [9]. Similarly, it is also present as a fibrous component in oatmeal and
a thickening agent in milkshakes in its modified form. Cellulose is a ubiquitous structural polymer
that will influence the strength of plant structure. As apparent from Figure 1, the unique properties
and high performance of natural fibers are influenced by their elementary nanocellulose fibers
components [10].
Research on cellulose is fueled by two possibilities: the chemical structure of cellulose as a
polymer, and the second is that cellulose contains crystalline domains that could be recovered using
chemical treatment. The second possibility of making cellulose crystals offers a further advantage of
developing nanocrystalline cellulose or nanocellulose with size-dependent properties[11]. These
natural fibers (restocked by the natural process of photosynthesis) represents about one-third of plant
cells. Research on nanocellulose has been undertaken worldwide, with the majority of work has been
carried out in the USA, Sweden, Finland, China, and India. The biosynthesis of nanocellulose
generates approximately 1,000 tons per year. Besides, nanocellulose is considered a viable alternative
to the more expensive high-tech materials such as carbon fibers and carbon nanotubes [12].
Subsequently, the nanocellulose market is projected to register to a value of $530 Million by 2021,
signifying the strong annualized CAGR of 25% between 2014 and 2021.
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Figure 1. Hierarchical structure of cellulose [8] [Reused with permission from the publisher].
Lauded as the “next wonder” material, cellulose boasts phenomenal versatility and
subsequently possesses a wide spectrum of characteristics. Nanocellulose, in particular, is
lightweight and concomitantly stiffer in comparison to Kevlar, rendering it exemplary as an
unprecedented armory[13]. It is also non-toxic, thereby opening up potential as additives and
preservatives for food-based products. Moreover, it offers tensile strength that is higher than steel by
eight-fold at similar dimensions. It is a plausible and sustainable alternative for the conventional
paper due to its lightweight properties and flexibility. Similarly, its buoyancy is unparalleled, as a
boat weighing one pound is capable of bearing cargo up to 1000 times heavier.
The nature of cellulose consists of both crystalline and amorphous phases [14]. In contrast to its
incredible strength, its crystalline form is characterized by a transparent material, especially a gel
containing microfibrils. As an advanced material, cellulose in its different state (e.g., nanofibers and
nanocrystal) are vigorously explored by the researchers due to its exciting behavior which promises
a wide range of application in electronic devices [3], material sciences [5], construction [7] and
biomedical sciences [8]. Nanocellulose with the properties of large surface area, hydrophilicity, sites
for chemical modifications; opens up their field for applications in industrial packaging, electronic
devices, cosmetic and medical devices [15-17].
In relation to nanocellulose research, a number of reviews have been carried out. Thomas et al.
[13] have reviewed and reported the challenges and recent developments in nanocellulose. They have
classified nanocellulose as a nanomaterial with excellent mechanical properties and biocompatibility.
Dhali et al. [3] reviewed the current status of industrial-scale production of nanocellulose and surface
modification techniques for nanocellulose. Guo et al. [14] comprehensively scrutinized the progress
of electrochemical energy storage of nanocellulose. Al-Oqla and Rababah [15] reviewed the design
challenges of preparing nanocellulose composites. Li et al. [16] focus on manufacturing food-grade
Pickering emulsions using nanocellulose, bacterial cellulose nanofibrils, and cellulose nanofibrils.
Currently, this nanocellulose is in more demand in 3D printing technology and food package
materials. Raghav et al. [17] reviewed nanocellulose for drug delivery applications. Guo et al.[6]
reviewed the research progress of nanocellulose in derived materials in electrochemical energy
storage.The present review is designed to cover the prospect that previous reviews have not covered.
Supplementary information (Table S1) summarizes and identifies the uniqueness of this paper
compared to others.
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From the above literature review, it can be declared that no review paper is available on the
sustainability of nanocellulose and its derivatives. This article aims to present a comprehensive
overview of the methods used for nanocellulose and its derivatives preparation, structure-property
and highlights the processing-property correlations and application of nanocellulose and its
nanocomposite materials. In the next section (Section 2.0), we provide a brief description of the
classification of nanocellulose. The objectives of this article are as the following: i) to differentiate the
classification of nanocellulose numbers; ii) to provide a brief account of the production methods that
have been developed for isolating nanocellulose; iii) to highlight a range of unique properties of
nanocellulose that have been extracted from different kind of experiments and studies; iv) to
elaborate nanocellulose potential applications in various areas. The final section concludes with final
remarks on the directions towards which future research on this new member of green technology
nature-based materials might be directed.
2. Classification of Nanocellulose
This section provides a brief description of the classification of nanocellulose – there are three
main classes, which are cellulose nanocrystals (CNC), cellulose nanofiber (CNF), and bacterial
nanocellulose (BNC). Considering the enormity of data, cellulose nanofibers developed by a scalable
top-down procedure, i.e., electrospinning, are also included in nanocellulose classes.
Two types of nanocellulose, CNC and CNF, are extracts from plant resources, such as wood,
while bacterial nanocellulose (BNC) is mainly obtained from living organisms by the process of
biosynthesis [15, 16]. The behavior of CNF is classified by the crystalline and amorphous percentage
of cellulose chains, while the CNC is crystalline domain cellulose. Figure 2 shows the SEM images of
the three main types of nanocellulose. Table 1 tabulates the three main classes of nanocellulose with
their typical resources, general formation method, and their size arrays.
Figure 2. Scanning Electron Microscope (SEM) images of three types of nanocellulose : (a) cellulose
nanocrystals [18], (b) cellulose nanofibrils [19], (c) bacterial nanocellulose [20] [Reused with
permission from publisher].
Table 1. The Classification of Nanocellulose.
Type of
Nanocellulose
Synonyms Typical Sources
Formation and
average size
Cellulose
nanocrystals (CNC)
Cellulose
nanocrystals,
crystallites, whiskers,
rod-like cellulose
microcrystals
Ramie tunicin, wood,
wheat straw,
mulberry bark
Method used: Acid
Hydrolysis.
Ø=5-70 nm
L=100-250 nm
Cellulose nanofibrils
(CNF)
Micro fibrillated
cellulose, nanofibrils,
and microfibrils
Sugar beet, hemp,
wood, flax
Mechanical treatment
and chemical
treatment
(a)
(b)
(c)
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Ø=5-60 nm
L=several
micrometers
Bacterial
Nanocellulose (BNC)
Bacterial cellulose,
microbial cellulose,
bio-cellulose
Low molecular
weight sugar and
alcohols
Bacterial based
approach
Ø=20-100 nm
2.1. Cellulose Nanocrystals (CNC) or Nanocrystalline Cellulose (NCC)
CNC usually serves as a reinforcing agent in a various field of applications, including improving
nanocomposite's mechanical strength and acting as a barrier material to reduce water vapor
transmission and oxygen gas [21]. CNC shows improved mechanical properties with greater elastic
modulus than Kevlar [22] and has a liquid crystalline behavior due to its asymmetric rod-like shape.
For biopolymer application, CNC is being explored to replace chemicals with petroleum base in green
technology evolution. With its interesting properties, CNC and its derivatives have been developed
for the following purposes;water treatment technology [23]. nanofillers for polymer matrices [24, 25],
templates for photonic hydrogels [26, 27], emulsifier for pickering emulsions [28, 29], and
mesoporous materials for biomedical fields [30]. CNC-based thin films have revealed to show its
interesting applications in oxygen barriers [31], anti-reflection coatings [32], enzyme detection [33],
and anti-counterfeiting [34].
2.2. Cellulose Nanofibrils (CNF) or Nano Fibrillated Cellulose (NFC)
The CNF being micrometer-long, consists of both amorphous and crystalline regions, different
from CNC, which are crystalline dominant. Usually, the synthesis of CNF can be done by mechanical
treatment such as grinding, milling, and homogenization or chemical treatment (e.g., TEMPO
oxidation), or both [35]. CNF is ideally used for medicine, optical, and reinforced composite
applications due to its renewability and biodegradability behavior and its amazing mechanical
behavior [36]. Recently, CNF serves as a dry reinforcing agent in paper industry applications,
suspension stabilizer and as a low-carb thickener [37]. The processed CNF have excellent mechanical
strength compared to polypropylene and polyester – old method man-made fibers. Also, cellulose
fibers can serve as a stabilizing crack, due to its close-spaced arrangement and high length-to-
diameter ratios [38].
2.3. Bacterial Nanocellulose (BNC)
BNC (average diameter in the range of 20-100 nm with micrometer lengths) are microorganisms-
based nanocellulose isolated from Gluconacetobacter - most efficient amongst cellulose-producing
microorganisms. BC is synthesized as pure nanocellulose and does not require any pre-treatment
procedures to eliminate lignin and hemicellulose[39]. Furthermore, it is a polysaccharide that is
frequently utilized in the food manufacturing field [40, 41], production of reinforced paper [42] and
broadly studied by scientists for medicinal and therapeutic purposes. This is evident, in the
multitude of in vitro and in vivo research that had revealed its biocompatibility [43, 44]. Similarly, its
outstanding mechanical performance encompassing water sorption capacity, porosity, stability and
conformability resulted in its extensive usage in cartilage tissue engineering [45], blood vessel
substitution in rats [46], and in wound healing [47].
BNC can be described as pure cellulose and unassociated with any other constituents[48]. BNC-
based nanocellulose composites are typically producible via the synthesis of BNC gel to alter its
cellulose biosynthesis. In contrast, BNC nanocomposites that are geared for biomedical applications
with enhanced mechanical characteristics are produced by BNC being soaked on polyacrylamide and
gelatin solutions [49, 50]. Meanwhile, BNC-hydroxyapatite scaffolds meant for bone regeneration are
fabricated by BC gel immersion, either in a simulated body fluid (SBF) or in both calcium and
phosphate solutions [51].
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Comparing CNC and CNF, bacterial nanocellulose has higher purity and crystallinity. These
nanocellulose has a high modulus (100-130 GPa), low density (1.5–1.6 g cm−3), tensile strength in the
range of 1.7 GPa, great water holding capacity, and biocompatibility [51]. Besides, various reports
indicated that BNC membranes fabricated with carboxymethylcellulose (CMC) displayed superior
metal ion adsorption capacity in comparison with pure BC membranes [52]. Electro spun cellulose is
a secondary class of nanocellulose developed from the main class of nanocellulose using an
electrospinning machine. The properties of the developed electro spun nanocellulose can be differed
by manipulating the process parameters.
3. Production of Nanocellulose
Production of nanocellulose from plant fibers usually involves chemo-mechanical treatments,
chemical methods, mechanical methods, and physicomechanical methods. Nanocellulose can be
naturally isolated via mechanical treatment and/or chemical treatment due to its natural hierarchical
structure. Figure 3 classifies the production method for nanocellulose.
Figure 3. Preparation methods for nanocellulose.
3.1. Mechanical Method
3.1.1 . Homogenization
Homogenization is one of the efficient methodologies for biomass refining due to its
effectiveness and simplicity. In addition, organic solvents are not generally required for
homogenization [53]. This method requires two types of equipment which are homogenizer and
microfluidizer (Refer to Figure 4). These apparatus are usually and widely utilized in the
pharmaceutical, cosmetics, food manufacturing, and biotechnology industries, and among others
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[54]. The homogenization procedures necessitates passing a raw cellulose resources via a very small
channel from the valve to the impact ring, which subsequently subjects the raw cellulose resources
to crush that ultimately guarantee nanocellulose formation.
Li et al. [55] synthesized sugarcane bagasse-based nanocellulose via a high-pressure
homogenizer. The homogeneous solution was transferred via a homogenizer without any clogging.
The isolation of nanocellulose involves 30 cycles pressurize procedure at the pressure of 80 MPa
under the optimum value (90%) of refining conditions. The obtained nanocellulose has a dimension
of 10-20 nm in diameter with reduced thermal stability and crystallinity compared to the original
cellulose.
Figure 4. Equipment used for homogenization process; (a) homogenizer (b) microfluidizer [Reused
with permission from publisher].
3.1.2 . Cryocrushing
Cryocrushing is a technique to fabricate nanocellulose fibers by freezing the fibers using liquid
nitrogen that undergo high shear forces process [56]. The use of the cryo crushing method is to
produce an ice crystal from within the cell wall, whereby the ice crystal forms of fibers underwent
high impact crushes resulting the breaking down and thereby liberating microfibrils [57].
Bhatnagar and Sain [58] successfully fabricated 5-80 nm nanocellulose fibers with a by the cryo
crushing method, as shown in Figure 5. The procedure involves dispersion of the cryo crushed
nanocellulose in a water suspension, incorporating a disintegrator prior to high-pressure fibrillation.
Wang and Sain integrated the combination of cryo crushing and high-pressure fibrillation processes
to produce 50-100 nm diameter of CNF by using soybean stock as the raw material [59, 60].
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Figure 5. Sample of cryo crushing system [Reused with permission from publisher].
3.1.3 . Grinding
Ultra-fine friction grinding with a specially designed disk has been used by several scientists to
produce cellulose nanofibers. In this process, the course raw cellulose will undergoes the static
grinding process and 1,500 rpm rotating grinding process. During the process, the brake down
process of cell wall of nanofibers composition will tahe place and the shear force from the grinding
process will fragment the H-bonds, producing of individualized nanofibers from the pulp [61]. Figure
6 presents the grinding equipment for nanocellulose isolation procedure.
Taniguchi and Okamura [62] have successfully formed 20-90 nm diameter of nanocellulose
fibers through the versatile super-grinding process. Meanwhile, the study by Iwamoto et al. [63]
subjected homogenized cellulosic pulp to the grinder treatment, yielding a bundle of fibers. The
procedure has come out with a uniform size of nanofibers in the range of 20-50 nm, after up to five
passes through the grinder, and with additional passes, the size of the fibrillated pulp fibers does not
change. In another article, Wang et al. [64] used a commercial stone grinder to synthesize CNF from
bleached eucalyptus pulp. SEM and TEM analysis revealed that the synthesized CNF was highly
kinked, had naturally helical and untwisted fibrils that serve as backbones of CNF networks.
Figure 6. Isolation of nanocellulose: Grinding equipment [64] [Reused with permission from
publisher].
3.1.4. Micro Fluidization
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Microfluidizer is another instrument that can be used to isolate nanocellulose fibers. Figure 7
shows the schematic diagram of the microfluidizer. Microfluidizer consists of the interaction chamber
and intensifier pump. The chamber is used to defibrillate the fibers while the pump serves as a
pressure controller. The fibers were defibrillated via shear and impact forces against colliding streams
and the channel walls inside the interaction chamber [65].
Lee et al. [66] studied the influence of the passing periods of MCC via microfluidizers on the
behavior of nanocellulose fibers. The aspect ratio of the nanocellulose fibers was found to increase
with the increase of cycles. Increasing further the passing times (up to 20 times) has caused in
agglomeration resulting from an increment of OH-groups and surface area of obtained nanocellulose.
These findings concluded that the number of cycles subjected to the homogenizer would yield CNF
with a higher surface area [66]. Similarly, the morphological analysis also indicated that nanofibers
of more homogenous size distribution could be produced by micro fluidization.
Figure 7. Schematic diagram of microfluidizer [64] [Reused with permission from publisher].
3.1.5 . Refining
The refining approaches, commonly practiced in the manufacturing of paper production. The
process involved the immersion of fibers in a based fluids medium until the cell wall of fibers swells
and peels itself, resulting the significant improvement in volume and specific surface area [67], while
also improving the microfibrils' accessibility in case of extended biological or chemical processes.
This renders it a typical process undertaken before big-scale CNF operations and production.
However, increments and decrements of the number of fines during the procedure will decrease the
fiber length. Figure 8 shows the schematic diagram of refining surfaces.
There are some devices utilized during the preliminary phases of CNF production to refine
cellulose, namely disk refiners [68, 69], PFI mills [70-72], and Valley beaters [73, 74]. Moreover,
grinders are also heavily referenced in reports as an instrument used to refine pulp before intensive
mechanical integration of a higher degree [75, 76]. Such a technique has also been evaluated as a sole
mechanical process for CNF isolation.
Disc refiners and their usage has been studied by Karande et al. [77], specifically in disintegrating
0.5% weight percentage of cotton fibers dispersed in water which had successfully reduced the
diameter of nanocellulose from 250 nm to 242 nm. The disintegration procedures occur alongside DP
decrement from 2720 to 740 and a decreased cellulose crystallinity. Refining approach is a frequently
used method as a mechanical pretreatment process during the initial phases of CNF isolation.
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Figure 8. Disc refiner opened to show the refining surfaces [78] [Reused with permission from
publisher].
3.1.6 . Blending
Uetani and Yano [79] demonstrated nanocellulose fibers isolation using a high specification
blender from softwood pulp, yielding uniform fibers of 15-20 mm diameter, as shown in Figure 9.
Their investigation looked into blending parameters under several isolated conditions, which
included cellulose concentration, stirring speed, and stirring duration. Cellulose pulp suspension was
found to be optimally processed at the concentration of 0.7 weight percentage at rpm of 37,000,
specifically in the context of nanocellulose isolation via this technique.
Moreover, a similar isolation technique using rice straw-based nanocellulose fibers was
demonstrated by Jiang and Hsieh [80]. The autbors mixed and crushed the fibers at the speed of
37,000 rpm with a heating temperature up to 97 0C for 2 hours. The experiment resulted in the
nanocellulose fibers with a bimodal size distribution. (Ø= 2,7 and 8.5 nm, L= 100-200nm).
Chaker et al. [81] used the pulp of high hemicellulose to prove the possibility of isolating
nanocellulose fibers. This was explicitly achieved by blending two-weight percentages of cellulose
for 20 minutes, resulting in a comparable yield value by comparing it with suspension passed for ten
cycles at a pressure of 600 bar in a homogenizer. Meanwhile, Nakagaito et al. [82] successfully
improved the effectiveness in minimizing the blending period by inventing a new blender bottle.
Figure 9. High-speed blender. The stainless-steel bottle has a 4-blade propeller and an undulated
inside wall [79] [Reused with permission from publisher].
3.1.7. Ball Milling
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An alternative method was introduced in the context of CNF production recently, namely ball
milling. This particular technique consists of a cellulose sample placed in a special bowl partially
filled with zirconia balls, as illustrated in Figure 10. The high energy collision occurs between these
balls resulting in cellulose disintegration, specifically during the rotation of the container[83].
Zhang et al. [84] have reported CNF isolation processes from softwood kraft pulp suspension at
a one-weight percentage concentration via this technique. The investigation focused on the influence
of isolation parameters such as zirconia ball size on the nanocellulose properties. The author found
that to prevent the recrystallization of nanocellulose, control of the isolation process condition is
needed.
Kekäläinen et al. [85] studied the isolation of nanocellulose fibers from hardwood kraft pulp via
the ball mill method. The effect of the grinding period, amount of fluid, and carboxylic charge
towards disintegration procedures and CNF properties were subsequently investigated in their
work, yielding substantial output. Discrete nanocellulose fibers of 3.2 nm diameter were produced
alongside nanofibril bundles of diameters ranging between 10-150 nm. Hence, such a method
remains to be challenged by the issues of quality and homogeneity of the isolated nanocellulose
fibers.
Figure 10. Scheme of the all-dimensional planetary ball mill [86] [Reused with permission from
publisher].
3.1.8. Aqueous Counter Collision (ACC)
ACC is yet another mechanical method elucidated for nanocellulose isolation, in which two
high-pressure jets of aqueous suspensions containing cellulose are impacted by one another[87], as
shown in Figure 11. Kose et al. [88] isolated discrete CNF via this method by using a homogenized
aqueous suspension containing a 0.4 weight percentage of bacterial cellulose. The jets of aqueous
suspension at a pressure of 200 MPa were processed for 80 passes, resulting in CNF with 30 nm
diameter. This technique also successfully produces CNF from microcrystalline cellulose [89],
measured at a length of 700 nm and diameter of 15 nm. However, as the precaution to prevent
clogging at the nozzle section, the dimension of the cellulose slurry must be smaller that the
diameter of nozzle channels.
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Figure 11. Schematic view of the aqueous counter collision (ACC) method [90] [Reused with
permission from publisher].
3.2. Chemical Method
3.2.1. Acid Hydrolysis
Acid hydrolysis is one treatment procedure for nanocellulose sources, which involves breaking
down the polysaccharides into simple sugar using acid solutions[91]. The acid hydrolysis process is
illustrated in Figure 12. For example, acid hydrolysis treatment can yield lignocellulosic fibers flax
(typically containing 20% to 40% hemicelluloses) as monomers. Hemicelluloses are more prone to
oxidation and degradation due to the more amorphous properties compared to cellulose. The
hydrolysis process may be faster when the pH value is reduced. For the acid hydrolysis procedure,
hydrochloric and sulfuric acid may be used for nanocrystal production. Hydrochloric acid yields
almost neutral nanocrystals of minimal dispersibility in water, whereas sulfuric acid generates
products of higher stability across a broad spectrum of pH [92]. The hydrolysis process places key
importance upon the reaction time, whereby an example is indicated by lengthy reaction time
bringing about complete cellulosic hemp fiber digestion. In contrast, inadequate and short reaction
period causes the large fibers generations and agglomerations not to disperse.
Figure 12. Schematic of nanocrystalline cellulose extracted from cellulose chains using acid
hydrolyzed [93] [Reused with permission from publisher].
3.2.2. Alkaline Pre-treatment
Alkali pre-treatment (Figure 13) involves eliminating the lignin, wax, and oils found on the
external surface of the plant cell wall as a cover. The treatment removes a certain amount of the lignin
structure and aids in the separation of the structural linkage present between the lignin and
carbohydrates [59, 60, 94, 95]. This is achieved using sodium hydroxide (17%–18%), which is
comparable to cotton mercerization. Furthermore, mild alkali treatment allows purification to occur,
resulting in insolubilization of pectin, hemicellulose and lignin. Nevertheless, alkaline pre-treatment
is subjected to careful control to prevent unwanted cellulose degradation and warrant hydrolysis that
only occurs on the fiber surface, ensuring the extraction of intact nanofibers [58, 59]. Similarly, some
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scholars opted for alkaline-acid pretreatment prior to the nanocellulose crystal mechanical isolation,
leading to lignin, hemicelluloses and pectin solubilitization [58, 94, 96].
Alemdar and Sain [96]also demonstrated such treatment to yield boosted cellulose amount for
wheat straw CNF, increasing it from 43 to 84%. It also revealed partial elimination of lignin and
hemicelluloses from wheat straw and soy hull fibers. Their respective nanofiber diameters ranged
between 10–80 nm and 20–120 nm. The nanocellulose production was sourced from pretreated fibers
via cryo crushing and fibrillation methods.
Figure 13. Deconstruction of lignocelluloses into cellulose, hemicellulose, and lignin [97] [Reused with
permission from publisher].
3.2.3. Oxidation Pre-treatment
Isogai et al. [98] introduced the approach of TEMPO radicals as an oxidative pre-treatment
before mechanical treatment takes place. The aggregation problem can be solved by TEMPO-
mediated oxidation as the technique guarantees surface modification via the introduction of COOH-
groups and CHO-groups into the solid native celluloses, subject to aqueous and mild conditions [19,
99]. Oxidation that occurred at the surface of the nanocellulose becomes negatively charged and
consequently causes the nanocellulose fibers to be repulsed, ultimately alleviating fibrillation.
3.2.4. Enzymatic Pre-treatment
The enzyme is good for lignin and hemicellulose modification and degradation process while
maintaining the portion of cellulose [100]. Many experiments had been done on the isolation of
nanocellulsoe fibers via enzymatic pretreatment [70, 101-103]. Pääkkö et al. [104] used enzymatic pre-
treatment in combination with homogenization and refining it to isolate softwood pulp-based
nanocellulose fibers. These authors revealed the following in their findings: a more significant aspect
ratio and lesser aggressiveness than acid hydrolysis in opting for mild hydrolysis using single-
component endoglucanase enzyme.
Furthermore, CNF fibrillation attempted by Janarchnan and Sain [94] had encompassed the
combination of bio-treatment with OS1, fungi isolation from elm tree infected with Dutch elm
disease, and high-shear refining upon bleached kraft pulp. The resulting TEM micrographs revealed
that more than 90% of the bio-treated nanofibers were characterized by a diameter less than 50 nm.
Similarly, they also depicted a higher aspect ratio and distinct characteristics in comparison to the
untreated nanofibers. Additionally, bio-treatment could increase the structural disorders seen in the
crystalline region, which enhances internal defibrillation.
3.2.5. Ionic Liquid
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Ionic liquids (ILs) are thermally and chemically stable fluids with low vapor pressure and non-
flammability organic salts with operating temperatures less than 100 °C [105-107]. They are widely
synonymous with dissolving cellulosic materials [108, 109]. Li et al. [55] used 1-butyl-3-
methylimidazolium chloride as an IL with HPH to generate sugarcane bagasse-based nanocellulose
fibers. It is obtained by dissolving the cellulose using IL, which passes through the homogenizer
easily without clogging. The cellulose precipitation occurs via addition of water and subsequently,
freeze-drying that generates the CNF. Consequently, it was found that cellulose solubilization was
influenced by several factors, namely the weight ratio of cellulose to ILs and the power of the
microwave and reaction temperature. The best solubilization output was observed at a reaction
temperature of 130 °C, 400W microwave power, and a 1% (g/g) cellulose to ILs ratio.
3.3. Physico-mechanical Treatment
3.3.1 . Ultrasonication
High intensity ultrasonication (HIUS) waves may cause great mechanical oscillatory power
secondary to cavitation. This is a physical occurrence encompassing the generation, growth, and
breakdown of microscopic gas bubbles upon the absorption of ultrasonic energy by molecules in a
liquid[110]. Figure 14 illustrates high intensity ultrasonication. The cavitation bubble and its
immediate area around reveal the production of volatile shock waves, thus resulting in implosion
sites characterized by temperatures reaching 5000 °C and pressures exceeding 500 atm. Therefore,
ultrasonic radiation is commonly utilized in various processes, including emulsification, catalysis,
homogenization, disaggregation, scission, and dispersion [111].
Extraction of nanocellulose from plant sources can also be done via HIUS energy in a bath
process. In this technique, the temperature of the nanocellulose fibers suspension increased
vigorously when the power was increased. A good amount of cellulose fibrillation can be obtained
when the temperature of the suspension is increased since the fibrillation of nanocellulose influences
the length of the raw fibers [112].
Figure 14. A typical laboratory rig for sonochemical reactions uses a high intensity ultrasonic [113]
[Reused with permission from publisher].
3.4. Chemico-mechanical Treatment
3.4.1. Steam Explosion
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Steam explosion is a break down process of structural elements of cellulose via thermo
mechanical approach. In this approach, lignocellulosic biomass is exposed to high pressure (in the
range of 35 bar) and moderate temperature (on the range of 423–503 K) for 1–20 mins in either a batch
or a continuous setup, as shown in Figure 15[114]. Steam explosion usuallu executed in a batch mode,
run for testing scale pre-treatment of continuous mode which usually applied for mass production
in manufacturing line.
Figure 15. Front and top view of the pressurizing vessel for steam explosion [115] [Reused with
permission from publisher].
3.5. Summary of Other Preparation Methods
Literature surveys reveal that nanocellulose is prepared from various natural resources by
several methods. Mechanical treatments mainly by homogenization, grinding, cryo crushing,
ultrasonication, steam explosion, and oxidation method successfully isolates nanocellulose with
diameters ranging from 10 to 80 nm. In contrast, chemical methods such as acid hydrolysis are used
to eliminate the amorphous regions of fibers and isolate CNC. All these treatments are expensive and
time-consuming as it involves high consumption of energy. For example, mechanical treatment may
cause a reduction in yield and fibril dimension as low as 100–150 nm, and it is not environmentally
friendly, same as chemical treatment procedures. The various preparation process, raw materials,
and their lengths are summarized in Table 2.
Table 2. Summary of various preparation method for nanocellulose.
Ref
Raw Materials
Preparation Method
Dimension
[116]
Cladodes of Opuntia
Ficus Indica
Homogenization ~ 5nm in width
[99]
Sugar beet pulp
TEMPO mediated oxidation
Not reported
[96] Wheat straw
Cryocrushing and
Homogenization
20-120 nm in width
[63]
Kraft pulp
Refining and Homogenization
50-100 nm in width
[117]
Cotton fibers
Refining
242 ± 158 nm in diameter
[118]
Sugarcane bagasse
Acid Hydrolysis
~32.84 nm
[119]
Cotton linter
Ultrasonication
15-35 nm in diameter
[120] Raw Cotton
Acid Hydrolysis and Alkaline
pre-treatment
Not reported
[121]
Cystoseria myricaas
algae
Acid Hydrolysis 10-30 nm
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[122] Hibiscus cannabinus
Alkaline pre-treatment and Acid
Hydrolysis
mean diameter of
6.1 ± 5 nm
[123]
Imperata
brasiliensis grass
Acid Hydrolysis
diameters were 10–60 nm
and length 150–250 nm.
[124]
Amylose maize starch
Electrospinning
1-4 μm in diameter
[125]
Apple and carrot
pomaces
Ultrasonication 3.31-3.54 nm
[126]
Peach palm extraction
(Bactris gasipaes)
Delignification treatments Not reported
[127] Moso bamboo culms
Microwave liquefaction and
Ultrasonication
567 ± 149 μm in diameter
[128] Areca nut husk
Acid Hydrolysis and
homogenization
1-10 nm in diameter
[129] Sugarcane bagasse Acid hydrolysis
69-117nm in length, 6-
7nm in diameter
[130] Oil palm trunk Acid hydrolysis
7.67-7.97 nm in diameter,
397- 367 nm in length
[131] Banana peel
Alkaline pre-treatment and Acid
hydrolysis
7.6-10.9nm in diameter,
454.9-2889.7 nm in length
[132] Raw jute fibers
Alkaline pre-treatment and
steam explosion
~50 nm in diameter
Regardless, these two nanocellulose extraction techniques from plants are impoverished as they
are time-consuming and expensive. Moreover, they require high energy consumption due to
mechanical treatments and processes, resulting in dramatically decreased yields and fibril length up
to 100–150 nm. Additionally, they are environmentally damaging, specifically for chemical
treatments. Therefore, scientists nowadays focus and emphasize methods that offer environmentally
friendly conservation, high efficacy, and minimal costs for nanocellulose production. Very few
references are available about the systematic study of nanocellulose extraction methods' influence on
nanocellulose quality and its capability in reinforced nanocomposites.
4. Surface Modifications of Nanocellulose
Natural cellulose in its original form is inappropriate or unsuitable for particular applications
because of its large dimensions and lower stability. To obtain a more suitable structure, cellulose may
be modified physically or chemically, or biochemically[133]. There are various surface modification
strategies, and some important modification methods were shown in Figure 16. The nanocellulose
surface can be tuned chemically by physical interactions and biological approaches due to the
hydrophilic nature and the presence of OH groups on its surface [134]. Surface functionalization of
nanocellulose may be done before or after the manufacturing process. The changes result in the
development of desirable properties, which improve the efficacy of the materials for a specific
application. The surface of a nanocellulose material can also be tuned in terms of how it interacts with
foreign substances by incorporating some chemical functionality, as noted by polymeric matrices
with improved reinforcement. Table 3 illustrates the various effect of surface-modified nanocellulose.
Lu et al. [135] investigated the properties of hydroxyapatite modified nanocellulose dispersed in
polylactic acid (PLA). The structural properties of modified nanocellulose was confirmed via
transmission electron microscopy, Fourier transform infrared spectroscopy, and X-ray diffraction
analysis. The authors reported the mechanical properties and thermal stability of hydroxyapatite-
modified nanocellulose enhanced dispersed in PLA enhanced due to the improved and stronger
hydrogen bonding at the surface of modified nanocellulose[135].
Li et al[136] enhance a nanocomposite films bonding of nanocellulose dispersed in polyvinyl
alcohol (PVA) by transplantation process of polyacrylamide onto nanocellulose. FT-IR analysis
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confirmed the presence of strong H-bond on the interface of modified nanocelulose, while
thermogravimetric analysis reported the modified nanocellulose-PVA nanocomposites had
enhanced their thermal stability behavior[136]. In another research study on nanocellulose surface
modification, Tang et al.[137] reported the nanocellulose implanted with butyryl chloride and
cinnamoyl chloride had successfully improve their surface behavior and could stabilize oil-water
emulsions in a sample. Nanocelulose with a high surface charge density limits their ability to stabilize
in any based fluids and thus, the hydrophobic modification of nanocellulose could enhanced
wettability, resulting in lower interfacial tension. Below some vital surface modification processes are
discussed in detail.
Figure 16. Figure Surface modifications of nanocellulose.
Table 3. Effect of surface modified nanocellulose.
References
Effect of surface
modification on
various properties
Before surface
modification
After surface
modification Reason
[138, 139] Crystallinity of
nanocellulose
Lower crystalline
value
Enhance the
crystalline value
A greater hydrolysis
time disintegration or
remove the amorphous
phase and improve the
crystalline value
Surface
modificatio
ns of
Nanocellul
ose
Carbanylati
on
Noncovalen
t surface
modificatio
n
Etherificati
on
Sulfonation
TEMPO-
mediated
oxidation
Acetylation
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[140, 141] Toxicity of
nanocellulose Toxicity
As per the
ecotoxicological
evaluation, the
nanocellulose has
lower toxic and
lower
environmental
damage
Proinflammatory and
Cytotoxicity reactions
are minimizing toxicity.
[142] Specific surface area
Lower specific
surface area 950-
200
m2/g)
Excellent specific
surface area (250-
350 m2/g)
H2SO4 treatment
[143] Aspect ratio Low or medium
aspect ratio Higher aspect ratio
TEMPO oxidation
method
[144, 145] Mechanical property Poor mechanical
property
Enhanced rigidity,
strength,
toughness, barrier
features, and even
flame retardancy
Collagen-based
composite films
reinforced with CNCs.
[146] Thermal property
Lower thermal
expansion
coefficient due to its
higher crystallinity
and strength of
nanocellulose
network
Excellent thermal
property
H2SO4 hydrolyzed
method
[139] Rheological property
Tendency to shear-
thinning and
pseudo-plasticity
depends on the pH
of the environment.
Enhancement in
shear rate with
lower viscosity of
nanocellulose.
TEMPO-oxidation
method
[147] Stability dispersion
and agglomeration
Agglomeration and
clustering of
nanocellulose
problem
Minimize the
agglomeration
problem
Freeze drying or
supercritical dying of
CO2.
4.1. Noncovalent Surface Modification
Generally, the surface modification is done through the absorption of surfactants with
oppositely charged polyelectrolytes. So that the nanocellulose interactions are via electrostatic and
hyperbolic attractions, Vander Walls forced or hydrogen bonds. Heux et al.[148] modified cellulose
nanocrystals with surfactants containing mono and di-esters of phosphoric acid with alkylphenol
tails. These surfactant molecules formed a coating at the surface of cellulose nanocrystals about 15 Å,
and these coated cellulose nanocrystals dispersed well in nonpolar solvents. Zhou and Teeri [149]
developed a new method for cellulose nanocrystal surface modification based on the adsorption of
saccharide-based amphiphilic block copolymers. They coated cellulose nanocrystals with a
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xyloglucan oligosaccharide–polyethylene glycol–polystyrene triblock copolymer. In nonpolar
solvents, these cellulose nanocrystals had a high dispersion capacity.
4.2. Carbonylation
Carbonylation is a surface modification process of an isocyanate with hydroxyl groups available
at the surface of the nanocellulose to form a urethane linkage. The addition of an additional n-
octadecyl isocyanate to cellulose nanocrystals and nano fibrillated cellulose in a bulk reaction in
toluene at temperatures between 100 and 110°C for 30 minutes without the use of any catalyst
improves their hydrophobicity[150]. Figure 17 shows the modification of cellulose nanocrystals with
3-isocyanatepropltriethoxysilane (IPTS) in Dimethyl formide. This modification reduced the
hydrophilicity of nanocellulose surfaces, which are prone to react with a low amount of free hydroxyl.
Figure 17. Schematic diagram of carbonylation process of nanocellulose [150] [Reused with
permission from publisher].
4.3. TEMPO-mediated Oxidation
TEMPO-mediated oxidation method is one of the most used methods for surface modification
method. TEMPO-mediated oxidation converts the hydroxymethyl groups in the nanocellulose to the
carboxylic forms. It involves the use of constant nitroxyl radical, TEMPO, in the presence of NaOCl
and NaBr[151]. Figure 18 illustrates the TEMPO surface modification structure of nanocellulose. De
Nooy et al. [151] suggested this kind of approach involves oxidation of primary alcohols without
effected the secondary OH-groups exposure of the glucose before it converted into carboxylic acids.
The formation of carboxylic acids also donates from the conversion of stable nitroxyl radicals into
OH-groups prior to oxidation reaction[63, 152]. Habibi et al. [35]reported that TEMPO-mediated
oxidation CNCs derived from HCl hydrolysis of tunicate-derived cellulose fibers and found that
TEMPO-mediated oxidation did not affect the morphological integrity of the CNCs. Qing et al. [153]
combined multiple approaches in the formation of eucalyptus kraft pulp into nanocellulose. The
processes involves TEMPO-mediated oxidation, enzymatic pre-treatment, grinding and
homogenization approaches in an accurate order. We can simply said that TEMPO-mediated
oxidation in impanation of macromolecules by suing amidation in order to ensure continuously
charging of negatively electrostatic force to the surface of nanocellulose, resulting in good dispersion
stability than obtained after sulfuric acid hydrolysis. Also, Osong et al. [154] mentioned that TEMPO
is a high cost approach. Cheng et al. [3] analyzed TEMPO mediated oxidized CNCs from different
cellulose by one step ammonium persulfate (APS) hydrolysis and reached 81 percentage yield. It
was found that the uniform CNCs with dense surface concentration of carboxyl groups and diameter
of 35nm produced at optimum conditions 16h at 80°C.
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Figure 18. Schematic diagram of TEMPO-mediated oxidation process of nanocellulose [Reused with
permission from publisher].
4.4. Esterification
Esterification through carboxymethylation of nanocellulose is an efficient process of treating and
forming nano-fibrillated cellulose. Generally, esterification is accomplished by activating the
structural components of cellulose in diluted NaOH, and the hydroxyl groups are converted to
carboxymethyl moieties with monochloroacetic acid C2H3ClO2 or its sodium salt[155]. The dispersion
and capability of carboxymethylated NFCs powder functionalized with 1-hexanol in extruded PLA
(Polylactic acid) composites have been investigated by Eyholzer et al.[156]. Hasani et al. [157]used
the etherification method to show the grafted cationic surface modification of CNCs. It was reported
that Alkali-activated hydroxyl (–OH) moieties of the cellulose backbone reacted with the epoxide of
EPTMAC through nucleophilic addition, resulting to high dispersion stability of mixture with
thixotropic gelling behaviour. This approach has some disadvantages, such as using a toxic
halocarbon reactant and creating more hydrophilic cellulose fibers than the initial ones. Cationization
can also be used to add positive charges to the surface of cellulose nanocrystals[158].
4.5. Acetylation
Acetylation is one of the most straightforward and inexpensive methods[159]. Acetylation
improves the CNC in nonpolar polymeric matrices by removing of H-bonds at the interface of
nanocellulose[160]. This approach replace hydroxyl groups with acetyl groups by applying an excess
amount of acetic anhydride [161], as shown in Figure 19. The acetylation for surface modification of
nanocellusoe is executed by removing the hydrophilicity of naocellulose, and enhances the affinity
between nonpolar solutions and interface of nanocellulose. For cellulose nanocrystal, the extra
approachs of post-esterification and acid hydrolysis procedures may cause lead to the low
crystallinity and changed in surface morphology of the obtained final product. For example, the
crystalllinity of cellulose nanocrystals reduced from 80% to 45%, resulting from the acetylation
approach of nanocellulose derived from acid hydrolysis procedures[162]. As a result, further efforts
are being applied in order to hydrolyze cellulose's amorphous regions while simultaneously
acetylating the hydroxyl groups.
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Figure 19. Schematic diagram of acetylation process of nanocrystals [163] [Reused with permission
from publisher].
4.6. Sulfonation
Sulfonation is a technique for increasing the hydrophilicity of cellulose surfaces. Sulfuric acid
increase the rate of the hydrolysis of nanocellulose to produce cellulose nanocrystal in which the OH-
groups are substituted with sulfate half ester moieties[164]. This substitution enhances the ability of
nanocellulose to disperse in any based fluids by preventing the formation of H-bonds and exerting
electrostatic repulsion between anionic groups [54]. The substitution of sulfate ester groups for
hydroxyl groups prevents CNC aggregation and aids in producing a stable colloidal suspension[165].
Even when hydrolysis parameters are precisely regulated, producing cellulose nanocystals with a
bulk amount of sulfate groups by straight forward sulfonation has proven difficult[166]. As a result,
after sulfonation, further modification of CNCs needed to fabricate cellulose nanocrystals with high
composition of sulfate groups. Neutralization process with NaOH, on the other hand, improves the
thermal stability of the H2SO4 isolated nanocellulosic material. In comparison to pure H2SO4,
spherical cellulose nanocrystals are produced through the sonication process during hydrolysis with
H2SO4 and HCl, with low density-dependent sulfate groups and maximum thermal stability[167].
The addition of NaIO4 and NaHSO3 to nano-fibrillated hardwood pulp resulted in the formation of
sulfonated based NFCs with diameters ranging from 10 to 60 nm[168]. Luo et al. [169] designed a
straight forward approach of fabricating sulfonated cellulose nanofibers with a high surface charge
density and fibrous structural morphology assisted with chloro-sulfonic acid. The authors reported
the modified CNF obtained high zata potential value with significant dispersion ability in based
fluids. The authors suggested post the sulfonation approach be utilized to adopt the dispersion ability
of cellulose nanofibers so that they can be used in a variety of applications.
4.7. Summary of Nanocellulose Surface Modification
In this subsection, the various method of surface modification of nanocellulose was analyzed in
detail. It was found that the surface modification pointedly improved the nanocellulose’s tensile
strength, thermal stability and thermal modulus, indicated that hydroxyapatite modified
nanocellulose is an excellent reinforcing matrix for PLA. The most used modification is covalently
attached hydrophobic molecules to the nanocellulose hydroxyl group via acetylation, oxidation,
esterification, and silylation. Table 4 listed different methods of surface modification of nanocellulose,
their main findings, and their applications.
Table 4. Overview of cellulose modification methods, their key findings and their applications.
References Nanocellulose Method Key findings Applications
[170] CNC H2SO4
Hydrolysis
High metal absorbing
capability and good
regeneration capacity
Better nanocomposite to
remove the contaminant
from industrial waste
[171] CNC H2SO4 hydrolysis
Improved dispersion
and thermodynamic
wetting
Reinforcements for
hydrophobic materials
[148] Nanocellulose
Noncovalent
surface
modification
Dispersion ability
improved Thermal energy storage
[172] Nanocellulose sulfonation
Improving formation of
stable colloidal
suspension
Determine aviation
energies for the
dehydration process
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[158] CNC Esterification
Cationic charges over
the surface of
nanocellulose
-
[151, 173] CNF
TEMPO-
medicated
oxidation
Formation of stable
colloidal suspensions Thermal energy storage
[150] Nanocellulose Carbonylation Improve the cellulose
hydrophobicity Packing applications
[174] Nanocellulose Acetylation Improve the cellulose
hydrophobicity Packing applications
[175] CNF
TEMPO-
mediated
oxidation
Improved
hydrophobicity and
thermal stability
Thermal storage
5. Processing-property Correlation of Nanocellulose
Owing to its eco-friendly attributes, excellent mechanical properties, low density,
biodegradability, and large numbers of availability for renewable resources, nanocellulose
production and applications in composites materials have recently attracted increasing attention.
Different behavior of nanocellulose causes different reinforcement of nanocomposite properties. This
section discusses the unique properties of nanocellulose, including the mechanical properties, optical
properties, barrier properties, rheology properties, morphology, degree of fibrillation, electrical
properties, and biodegradability.
5.1. Mechanical Properties
The mechanical properties of nanocellulose are influenced by the morphological aspect,
geometry, crystal structure, and anisotropy and defects caused during manufacturing. The various
studies and various methods of mechanical properties are shown in Table 5. Taniguchi and Okamura
[62] synthesized CNF from different sources (cotton cellulose, wood pulp, and Tunisian cellulose) via
a simple mechanical procedure. The CNF then undergoes the homogenizing procedure by using
solvent casting to form translucent films with 3–100 μm thickness. The results obtained reveal that
the tensile properties of wood pulp-based nanocellulose and tunicin-based nanocellulose were
respectively 2.7 times more than that of polyethylene (PE) and 2.5 times more than standard grade
paper. However, these tensile properties, which were measured in the work, have not been explicitly
enumerated.
The mechanical characteristics of CNF films were also found to decrease upon immersion in
water, but with most of the structures retained. Their non-dispersibility in fluid features is
attributable to the high strength hydrogen bonding interaction present along side-by-side of the
nanofibers after drying processes. Furthermore, arbitrary in-plane CNF orientation notwithstanding,
these films display remarkable mechanical characteristics [176].
Zimmerman et al. [177] obtained nanocellulose fiber from sugar beet pulp chips using the
solvent casting method. The tensile obtained strength - nearly reaches the tensile strength of clear
wood in the range of 80-100 MPa with an elastic modulus of 6 GPa – the same results were also
obtained by Leitner et al. [178]. Also, these authors demonstrated wide-angle X-ray scattering on the
dried nanocellulose sourced to reveal the homogeneous azimuthal distribution of smattering
intensity, further substantiating CNF’s arbitrary inclination. These sugar beet-derived nanocellulose
generated 104 Mpa of tensile strength and 9.4Gpa of modulus of elasticity
Bruce et al. [179] obtained the tensile strength and elastic modulus of 100 MPa and 7 GPa from
their investigation, respectively. The nanocellulose sheet was obtained via a homogenized high-
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pressure method with the sources of swede root pulp. Another researcher, Dufresne et al. [180],
prepared nanocellulose fiber from sugar beet pulp and obtained significantly lower tensile strength
in the range of 2.5 – 3.2 GPa. Moreover, these scholars highlighted the stiffer conditions of the CNF
when pectin was present, which was one of the key components of pulp (25– 30 wt%).
Henriksson et al. [181] analyzed the influence of morphology on mechanical properties of pure
nanocellulose fibers by varying molar mass of cellulose parameters. Upon altering the morphology
of nanocellulose via the addition of solvents, SEM analysis reported a spider web-structure, fine and
remarkably fibrous morphology arrangement on the surface of nanocellulose. The SEM analysis also
revealed that the typical lateral dimension of nanocellulose was found to be in the range of 10-40 nm,
proving that their arrangement is made up of aggregated cellulose microfibrils instead of smaller and
discrete microfibrils.
Table 5. Mechanical Properties of Nanocellulose from previous studies.
References Raw material Preparation method Max. Stress
(MPa)
Modulus of
elasticity
(GPa)
[181]
Softwood dissolving
pulp
Vacuum filtering 104 14.0
[182]
Softwood and
hardwood bleached
kraft pulp
Vacuum filtering 222-233 6.2-6.9
[183]
Hardwood bleached
kraft pulp
Vacuum filtering 222-312 6.2-6.5
[184]
Bleached spruce
sulfite pulp
Vacuum filtering 104-154 15.7-17.5
[178]
Sugar beet pulp chips
Casting
104
9.3
[185, 186]
Ramie
Retting
393-870
7.3
[185, 187]
Cotton
Acidic hydrolysis
128-597
5.5-12.6
[188]
Kenaf
Retting
930
53
[189]
Jute
Retting
393-800
10-30
[190]
Banana
Chemical treatment
600
17.85
[191] Bleached birch pulp
Mechanical
disintegration
172 5.3
[192]
Bacterial
Nanocellulose
Not reported 357.3 20.8
[193]
A. xylinum
Two-step purification
88.9
7.6
[194]
Gelatin (A. xylinum)
Static cultivation
63
Not reported
[195]
Murlberry pulp
Acid Hydrolysis
33.3-41.3
0.77-1.11
[196]
Tossa jute fiber
Acid Hydrolysis
32.94 – 48.66
4.81-5.76
[197]
Softwood pulp
Ultrasonication
141.6
12.27
[197]
Algae
Ultrasonication
77.97
8.12
[198]
Cotton
Disc refiner
23-26
Not reported
5.2. Optical Properties
Reinforcing elements with diameters of less than 0.1nm of visible light wavelengths are not
expected to cause light scattering [202]. Cellulose nanofibers which proven in this size range; unless
significant nanofibers are densely packed, and the interstices between the fibers are small enough to
avoid light scattering, optically transparent nanocellulose in film form should be predicted.
Transparency of nanocellulose was improved by Siro and Plackett [199] by exposing the
preliminary nanocellulose gel to additional homogenization phases before the preparation process.
These phases may be as many as three, thus resulting in disintegrating nanocellulose fiber aggregates
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of larger size. Consequently, improved light transmittance was seen at 600 nm for 20 μm-thick films,
specifically from 61% to 82%.
Nogi et al. [200] investigated the influence of nanocellulose surface roughness on its
transparency. The nanocellulose transmittance is shown in Figure 20. The authors revealed the
significant decrease of light transparency of films with the increment of the light scattering
(wavelength). The polished nanocellulose films obtained about 90% of total light transparency after
impregnating via an optically transparent polymer layer[201].
Figure 20. Light transmittance of microfibrillated cellulose films [200] [Reused with permission from
publisher].
5.3. Barrier Properties
Theoretically, it is not an easy way to diffuse the molecules to penetrate with the crystal parts of
nanocellulose fibers [184]. The factor of having high crystallinity properties [202, 203] and the nature
of nanocellulose fibers to serve as a bulk network were held together by inter-fibrillar solid bonds,
suggesting that nanocellulose fibers might serve as a barrier material.
Fukuzumi et al. [182] concluded that the oxygen permeability of polylactide (PLA) films
improved by more than 700 times upon the addition of nanocellulose fiber layers to their surface.
This indicates these fiber’s highly hydrophilic characteristics and subsequent tendency to absorb a
notable amount of moisture. Nevertheless, their properties of water absorption and swelling
phenomenon were highly intricate to be explained. Still, they were postulated to be affected by the
arrangement of atoms of the cellulose and the film’s mesostructured alike. To the best of the author’s
knowledge, one sole work has so far pioneered in publishing and discussing the water uptake for
neat nanocellulose fibers films [203]. However, it is important to note that no findings regarding such
film’s water vapor permeability have been obtained. Thus, this allows the conclusion that the
addition of nanocellulose fibers reduces the water molecules absortion of potato starch-based
nanocellulose[204, 205]. However, the impact of density and porosity of nanocellulose on barrier
properties remains complex to explain.
Another researcher demonstrated noteworthy nanocellulose fiber porosity, which seemingly
opposed its high oxygen barrier characteristics. The researcher suggested that nanocellulose films
possessed a very tight pores in the centre of their cross-section, rendering the inference that their
oxygen barrier attribute was a consequence of close nanofiber order and pack. Additionally, it may
also be influenced by the crystalline properties of nanocellulose [181].
5.4. Rheology of Nanocellulose
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The rheological features were studied on nanocellulose crystal suspensions. In a “dilute” regime,
these nanocellulose crystal suspensions undergo the shear-thinning process, and the obtained
rheology properties improve as the concentration increases. Concentration correlation was notably
prevalent at low shear rates, while high shear rates revealed the opposite. The nanocellulose crystal
suspension is considered at lyotropic (high concentration condition) and causes anomalous
transitions to occur in the flow. This suggests their tendency to situate themselves at a critical shear
rate according to their rod-like temperament and, next, smoothening their flow at a higher rate. Such
changes and their rate of occurrence in the flow properties are notably concentration dependent.
Table 6 shows the various rheology results from the previous study.
Rheology of the nanocellulose fibers suspensions developed using TEMPO-oxidation also
revealed that the associated shear-thinning characteristics stemmed after power-law and thixotropy.
These elements are subjected to a discourse via percolation in the fibrils and flock establishment [206].
Another research regarding nanocellulose attributes also indicated that wood and bacterial
nanocellulose alike demonstrate a significant capacity for water storage [207]. Similarly, in the case
of a 2% solid content, its dispersion performance in the water also resulted in a transparent gel that
is mechanically substantial. This suggested that wood-based nanocellulose crystal prepared via
mechanical treatment seems to have reduced the Young Modulus in the range of 50 - 100 GPa [207]
than those of bacterial nanocellulose.
Table 6. Rheology Properties of Nanocellulose from previous studies.
References Raw material Shear rate (s-1) Viscosity
Run Temp
(
o
C)
[208]
Pineapple
22.2
3.5 x 10
4
Pa.s
125
[209]
Softwood sulphite pulp
20
260 mPa.s
20
[210]
Cellulose nanofibrils
0.1-1.0
10 – 100 mPa.s
25
[211]
Kenaf/PLA
10
3
-10
4
50-300 Pa.s
200
[212]
Jute/PP
10
-2
-10
4
10 – 10
4
Pa.s
180
[213]
Hemp/PP
10
-1
-10
3
10
2
-10
5
Pa.s
180
[214]
Gluconacetobacter xylinus
0-400
170-400 Pa.s
25
5.5. Morphology
The morphology structure of nanocellulose generated is undoubtedly one of the critical
properties capable of modulating the production processes. Therefore, the sources and
manufacturing procedures of cellulose are significant because CNF morphology strongly depends
on them. Besides, if dissimilar microscopy methods and sample preparation methods are utilized for
the analysis, the observations can be slightly different. For example, some dehydration procedures
may result in CNF aggregation to a certain degree [54].
In the study conducted by Henriksson et al. [72], homogenization and enzymatic hydrolysis of
bleached wood sulfite pulp served to generate 5-30 nm diameter of nanocellulose, obtained from
AFM analysis. In contrast, Liimatainen et al. [215] substantiated the production of CNF of 3-5 nm
diameter via periodate chlorite oxidation and subsequent homogenization. TEM analysis also
measured the diameter of 3–5 nm.
Olszewska et al. [216] agreed that CNF obtained via homogenization and quaternization
revealed a diameter ranging from 2.6–3.0 nm as inferred using TEM. Hence, CNF of 3-5 nm diameter
may be attributed to the elementary fibrils, whereas thicker diameters may represent elementary
fibril bundles (generally microfibrils).
Because of the high aspect ratio of nanofibrils, the determination of CNF length becomes
problematic. For a comparably high magnification case, the diameter of a cellulose nanofibril is
identifiable, while its length had exceeded beyond the measurement range. Additionally, decreased
magnification undertaken to capture the entire length will result in nanofibrils that cannot be
detected because of the small diameter.
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In conclusion, the introduction of charge groups may be notably attributed to the production of
CNF of a smaller diameter. Besides, CNF is mechanically delaminated and enzymatically
hydrolyzed prior to being associated with more entanglement and flocculated structures, as depicted
by Nechyporchuk et al. [217]. The material generated is typically characterized by a section of non-
fibrillated microscopic fibers or fiber chunks other than the nanofibrils.
5.6. Degree of Fibrillation
Usually, the morphology of the CNF is determined by the synthetic protocol. A microscopy
technique is used to corroborate the existence of nanofibrils in the materials generated. Nevertheless,
this particular investigation may eliminate the remaining microscopic fibers and fiber fragments.
Other than that, the concept of “degree of fibrillation” is also required to calibrate the cellulose
molecules as carrying out microscopy characterization at varying magnifications. It is also a time-
consuming process. This is further compounded by the need to ensure repeated quantification to
generate diagnostic findings.
Calculating the yield of fibrillation [218] is one of the methods undertaken to assess the extent
to which fibrillation occurs. The suggested technique entails centrifugation of a cellulose suspension
with a weight percentage in the range of 0.1–0.2 at 4500 rpm for 20 minutes, despite the instrumental
details or relative centrifugal force were unnamed. This step will isolate the CNF in the sedimentation
from the non-fibrillated residue. The CNF suspensions and films' capacity to emit or disperse visible
light will also elucidate with the degree of fibrillation, as light dispersion is more in the case of more
microscopic fibers and their fragments that have sustained their form in the suspension. This will
inevitably yield CNF suspensions or films that are less transparent, thus rendering the commonly
utilized ultraviolet-visible spectroscopy used to test both CNF suspensions [98, 168, 218] and films
[153, 219].
Syverud et al. [184] incorporated a desktop imager scanner to assess nanocellulose film
transparency. Meanwhile, Chinga-Carrasco [220] differentiated various optical methods to quantify
the degree of CNF fibrillation in suspensions and films. They included ultraviolet-visible
spectroscopy and turbidimetry and a multitude of devices like image scanners, fiber optic testing
apparatus, and a light source digital camera system to obtain dynamic values. These optical methods
and tools were detailed to be appropriate in quantifying CNF suspension and film light
transmittance, which was impacted by surplus residual non-fibrillated fibers. Regardless, the image
scanner was deemed as the most suitable in assessing the degree of fibrillation for CNF films as its
fiber residues are easily identifiable. Besides, the light source–camera system for dynamic
measurements was also performed according to a review of the grey level of the images, which
displayed a promise for concomitant investigation of the degree of fibrillation in CNF production
processes.
5.7. Electrical Properties
Nanocellulose nanoparticle utilization in conductive materials is an excellent idea as an
alternative for carbon black-based nanocomposites. Recently, a substantial amount of efforts were
expended on the fabrication of conductive paper and ink, parallel to their potential role as a
component of batteries and electronic displays [221-223].
The first examination on nanocellulose crystal conductivity had tried to determine the
accessibility of a percolated network of particles. Flandin et al. [224] secured the nanocellulose crystal
particles with conductive polymer polypyrrole before bringing the samples into a poly (S-co-BuA)
latex lattice. The investigation proved that conductivity had started in the material after
accomplishing a critical volume fraction of particles, which neared the volume of particles
tantamount with the percolation threshold computed.
Similarly, Schroers and colleagues [225] implemented nanocellulose crystal particles combined
with ethylene oxide-epichlorohydrin as a matrix to get its conductivity with great mechanical
behavior. The technique of nanoparticle coating with conductive polymers was also explored further
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in other varying reviews, with additional cases being fabricated with high conductive nanocellulose
via PANI-modified BC. The resulting materials were found to display flexibility and excellent
conductivity of 5.0×102 S/cm [192]. The various types of cellulose and their electrical properties are
shown in Table 7. Meanwhile, Cao et al. [226] hybridized graphene sheets with nanocellulose crystal
in water suspension prior to introducing hydrazine hydrate to reduce the particles. The ensuing
hybrid nanoparticles were amalgamated with NR latex and then dried to yield conductive materials.
Additionally, Wang et al. [227] suggested that CNC-based conductive materials be utilized as
an application for flexible strain sensors. The electric percolation threshold was lower by four-fold in
case of a 3D structure incorporated with CNC compared to a pure NR carbon nanotube
nanocomposite. These materials had demonstrated electrical responses upon being subjected to
wide-ranging tensile strains.
Table 7. Electrical Properties of Nanocellulose from previous studies.
References
Nanocellulose type
Conductive structure
Conductivity (S cm
-1
)
[228]
CNC
PPy
Up to 36
[229]
CNF
PPy
1.5
[230]
CNC
PANI
Up to 10
-1
[231]
CNF
PANI
2.6 x 10
-5
[232]
CNF
silver
5
[233]
CNC
PANI + PFE
0.01 – 0.5
[234]
CNC
PPy
Up to 4
[235]
CNC
PANI
2.6 x 10
-5
[236]
BC
CNT
0.13 x 10
-3
[191]
CNF
GO
7.3 x10
-2
-15.4
[192]
BC
PANI
2.0x10
-4
-9.5 10
-3
5.8. Biodegradability
Polysaccharides like nanocellulose and starch may undergo degradation due to bacterial and
fungal strains. In contrast, a few selected general matrices polymers are only degradable by bacterial
strains (e.g., NR) or fungal strains (e.g., PLA) [227, 237]. Regardless, nanocellulose is characterized by
the role of the nanoparticles and matrix as a source of carbon for microorganisms, particularly if
moisture is present. Additionally, Abraham et al. [237] depicted the step-by-step biodegradation of
NR/nanocellulose, implying that the nanocellulose-reinforced phase had undergone degradation
before the pure NR material. Such exacting biodegradation of the nanocellulose-fortified component
over the NR part, while being subjected to identical experiment circumstances, is clear evidence of
the process being instigated in the nanocellulose-reinforced NR.
6. Applications of Nanocellulose
Recently, nanocellulose emerged as a potential commercial material, whereby despite its broad
spectrum of possible applications, more are being designed and visualized. Nanocellulose can even
be described as a solution looking for more problems to solve. If utilized as an automotive material,
it may be substituted for fiberglass to develop auto components that are 10% lighter, thereby
instigating comparable vehicle fuel consumption reduction. Moreover, it may be utilized to relieve
arthritic joints and the production of nano chitosan for immediate clotting and traumatic wound
healing either in a battlefield or emergency cases. This section outlines the main applications of
nanocellulose, as shown in Figure 21.
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Figure 21. Main Application of nanocellulose [Reused with permission from publisher].
6.1. Biomedical
CNC with high crystalline properties can contribute to a rigid surface and is associated with
tunable functional groups accessible for grafting and modification. Therefore, such unique properties
of CNC are very engaging for biomedical applications and suggested by scientists for being widely
used in medical science [238]. For example, modified CNC has been recommended to be used in
chemotherapeutical drugs [239] due to its form that is valuable for folic acid delivery treating brain
cancer tumors. Zoppe et al. [240] exposed CNC as viral inhibitors (alphavirus infectivity) and
recommended that it is also used for other viruses. Also, CNC has compatibility for biosensing and
detection, specifically for CNC-based biosensors via peptide conjugation to identify human
neutrophil elastase [241, 242].
The advantages of CNC in medical sciences and drug applications are primarily dependent on
its usage as a liquid. In contrast, for biomedical applications, it is preferred in solid-state[243].
Meanwhile, CNF is the key material for biomedical applications. CNF, with the criteria of not being
harmful in effect, having a large surface area, smoothness, and low porosity, makes it suitable as
substrates for biosensors (processed by attaching peptides to the support matrix). These substrates
that have spurred EDS/NHS chemistries have been proven to bind themselves to the bovine serum
albumin (BSA), subject to non-porous cellulosic films for diagnostics [244]. The modification of CNF
with reactive amine film is shown in Figure 22.
TEMPO-oxidized CNF (TOCNF) has been widely implemented to develop the support film with
carboxyl groups before being transformed into amine-reactive species. The substrates were then
utilized to bond with BSA and polyclonal anti-human immunoglobulin G (IgG). Another method
used - CNF surface, activated via co-polymer grafting to manufacture biosensors for BSA and
immunoglobulin G (IgG) detection. A peptide protein with a specific affinity to human IgG was
chemically combined with the grafted polymer to generate a highly selective binding system [245,
246]. The number of advantages highlighted accordingly has already underlined the potential for
additional material anticipated by everyone and the assumption for CNF to be prospective and
accessible for individuals in bioactive interfaces.
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Figure 22. Modification of CNF films with reactive amine groups for detection of biological species
[244] [Reused with permission from publisher].
6.2. Flexible Display
Wood-based nanocellulose composite can be a platform for developing display substrates due
to its optical transparency, flexibility, and low-CTE properties[247]. Advanced organic light-emitting
diode (OLED) is one example of a successful device designed in this application [248]. Figure 23
shows the flexible display using the CNF substrate. It successfully scaled the 21 ppm/K of CTE value
of cellulose substrate for OLED display. In contrast, transparent and flexible nanocomposites made
up of BC, and PU-based resin was fabricated recently as a substrate for OLED. It boasted a high light
transmittance of a whopping 80%, notable stability of up to 200 cd/m2, and CTE-based dimensional
stability as low as 18 ppm/K [249].
Figure 23. Flexible display on CNF substrate [250]. [Reused with permission from publisher].
6.3. Energy Storage
The morphological properties of nanocellulose make it a good alternative for energy storage
applications [251, 252]. The reduced porosity of nanocellulose exhibits its usage as a liquid electrolyte-
ionic transport between the electrode surface [253]. For energy storage application usage,
nanocellulose has been used with MWCNT to develop flexible energy storage gadgets [254]. The
application of thermal energy storage on CNF aerogel is shown in Figure 24. Its arrangement is simple
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and comprises one individual, thin conductive cellulose paper fabricated from ionic liquid at room
temperature while the MWCNT served as an electrode. The nanocellulose was also designed for high-
power batteries, specifically as electrolytes, electrodes, and separators. As a benefit, nanocellulose
based high power battery is a straightforward integrative procedure incorporating an individual
flexible paper structure [255].
In Li-ion battery (LIB) polymer electrolytes, various reports have highlighted the use of CNF
composite membranes with a significant Young’s Modulus of 80MPa, excellent ionic conductivity
(approaching 103 S/cm), and stability with an all-inclusive electrochemical performance [256]. The
latest update included a CNF composite with a liquid electrolyte with extremely high mechanical
strength and an ionic conductivity value for LIB application of approximately 5×10-5 S/cm [257].
Sun et al.[252] developed 3D polypyrole electrode doped with nanocellose (CNC) for energy
storage application. The research revealed that with the presence of nanocellulose, the 3D polypyrole
electrode have a more porous and hierarchical structure, as well as better electrochemical
performance. The porous morphology formation from the doping of polypyrole with CNC and
inorganic salts opens up more active reaction areas to store charges in polypyrole electrodes as the
stiff and ribbon-like nanocellulose that serve asdopants improve the strength and stability of PPy-
based films[258].
Zhu et al. developed a sodium-ion battery by utilizing wood-based nanocellulose as the
electrolyte. A nature of wood fibers exhibits mesoporous behavior that served as ion transportation
through the fiber. This successfully resulted in a high stability and great performance of battery cycles
with capacity of 339 mAh/g. The novel development is expected to be implemented for cost effective
sodium-ion-based batteries [259].
Figure 24. Energy-storage device assembly in a CNF aerogel by LbL technique [250] [Reused with
permission from publisher].
6.4. Paper Transistor
As the green technology and low-cost substrate in the semiconductor industry flourishes,
nanocellulose has been considered for the possibility as transparent insulation. The paper-based
transistor was previously highlighted due to its flexibility, disposability, and low cost, packaged as
biosensors, innovative packaging designed with the prerogative of organic semiconductors to be
compatible with paper substrates [260]. However, the proposed paper-based transistor is unable to
fill the role of silicon transistor because of the dimensional issue. Still, the fabrication is considered
cheap and for disposable applications. The printing method used to fabricate the paper-based
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electronics devices ensures the inexpensive and express manufacturing process using low-cost
disposable substrates from nature [261, 262].
Fujisaki et al. announced the creation of a nanopaper transistor made of native wood CNF
through lithographic and solution-based techniques, as shown in Figure 25. They created a
nanopaper transistor that has good flexibility and can be formed into an arbitrary shape. These
headway of green innovation and minimal effort paper substrates and solution-based natural thin-
film transistors are promising for use in the future for adaptable devices application [263].
Figure 25. (a) 20 μm thick of transistor nanopaper (b) bending state (c) folding state [263] [Reused with
permission from publisher].
In another research, Hassinen et al. [264], revealed entirely printed top-gate-bottom-contact
natural paper transistors by utilizing substrates arranged from CNF and monetarily accessible
printing inks to create the gadgets. Gravure printing was used to coat the substrate with a polymer
instead of diminishing the surface harshness and closing the surface. Transistor structures were
manufactured utilizing inkjet printing for conveyors and gravure printing for the dielectric and
semiconducting layers. They revealed that the transistor execution is contrasted with that of
comparable transistors on the plastic substrate.
6.5. Solar Cell
Nanocellulose is also a suitable candidate in solar cell application due to its being inexpensive,
high porosity, and flexibility that could enhance the express manufacturing way of solar cells [265,
266]. However, the fiber diameter for commercial papers exceeds the visible light wavelength,
rendering them non-transparent. However, some CNF fibers recorded diameters as low as 4 nm,
highlighting its remarkable candidacy in developing ultrathin paper solar cells.
Zhou et al. [267] fabricated effective solar cells utilizing nanocellulose crystal as the substrate.
They achieved positive rectification in the dark with high power efficiency of 2.7% and being
recyclable into single components using low-energy processes at ambient conditions. Then, Zhou et
al. extended their research for featuring solar cells with 4% efficiency of energy conversion. To
achieve that, they developed solar cells using a film-transfer lamination, whereby the CNC substrate
was deposited with conducting polymer.
Also, nanocellulose can be used as an extra mechanical component for solar cell systems.
Yuwawech et al. [268] specifically looked into improving the barrier, thermal, and mechanical
attributes for ethylene-vinyl acetate copolymer encapsulated solar cells, equipped with reinforced
esterified nanocellulose fibers. Regardless, this research displayed chemical modification of bacteria
nanocellulose using propionic anhydride before being intensified by EVA in a twin-screw extruder.
The introduction of CNFs has delayed the degradation of the EVA film via deacetylation while
retaining the EVA film's visible light transparency of above 75%.
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6.6. Overview of Nanocellulose Application
Nanocellulose holds a great prospect in many applications, including energy storage, paper
transistor, solar cell, flexible display, and biomedical applications. Undoubtedly, nanocellulose has
excellent potential to be used for the development of emerging devices and instruments for advanced
applications. We believe that several areas need to be addressed and plenty of possibilities to be
explored in this area. Table 9 had listed several examples of nanocellulose applications reported for
different types of cellulose materials.
Table 9. Example of nanocellulose application.
Ref
Class of
Nanocellulo
se
Raw materials Special Properties Field of application
[181] CNF Softwood Pulp High Toughness Nanopaper
[269] CNF Not reported Cell-friendly
3D Bioprinting Human
Chondrocytes
[270] CNF Oat Straw High Porosity
Selective Removal of
Oil from Water
[271]
BNC
Not reported
Natural Abundance
Energy Storage Device
[272] CNF
Bleached softwood
pulp Not reported
Organic Light Emitting
Diodes
[228]
CNC
Not reported
Not reported
Supercapacitor
[249] BNC
Nata de coco(A.
xylinum)
Flexible
Organic Light Emitting
Diodes
[273] BNC
Gluconacetobacter
xylinum
Not reported Drug delivery system
[274]
CNF
Not reported
Highly Stretchable
Strain Sensor
[266] CNF
Softwood Cellulose
fibers
Superior Optical
properties
Conductive paper
[275]
CNF
Not reported
High Porosity
Oil absorbent
[276] BNC Bacteria suspension
Good tensile
mechanical
properties
Ear cartilage
replacement
[239] CNC Bleached softwood
sulfite pulp
Oblong geometry,
lack of cytotoxicity,
numerous surface
hydroxyl groups
Chemotherapeutic
agents to cancer cells
[277] CNC Not reported
Eco-friendliness and
biodegradability
Anti-bacterial food
packaging
[198]
CNF
Cotton
Not reported
Food-packaging
7. Future Perspectives and Challenges
At present, nanocellulose is currently required to go through several phases of alteration in the
manufacturing process before its potential application, which necessitates the use of harmful
chemicals and high risk reaction. Future research should focus on developing simple and straight
forward procedures with less harmful conditions. During acid hydrolysis, extra caution is needed to
avoid structural damage. The harm can be minimized by implementing pre-treatment procedures;
however, several measures are expensive, limiting their commercial application. As a result, basic
techniques may be used to preserve and/or improve the morphological behaviour of final products
Low-cost and straightforward approaching should be at the the main objective for the future
development. One of the most important moves towards environmental sustainability is the
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preparation of nanocellulose by mechanical and chemical treatment processes that could produce
biodegradable green nanocomposites. Thus, researchers should focus and accentuate this method to
be environmentally friendly, inexpensive, and high efficiency for nanocellulose production. There is
currently a scarcity of adequate toxicity testing for extracted nanocellulose and modified
nanocellulose, which is critical for their unrestricted and extensive use. We hope that this analysis
will spur research into improving the manufacturing process and properties of nanocellulose, thereby
broadening their industrial applications and promoting the long-term use of renewable materials. As
a result, potential developments emphasizing cost-effective and environmentally sustainable
nanocellulose extraction and modification routes would encourage the rapid and favorable
development of this "wonder" biomaterial for various applications.
8. Conclusions
Nanocellulose is a sustainable, abundant biopolymer derived from various living species such
as plants, animals, bacteria, and amoebas. This review differentiates three main classes of
nanocellulose (CNF, CNC, and BNC). All these classes of nanocellulose are immediately accessible,
renewable, and sustainable, thus presenting themselves as green technology and promises of
amazing benefits in today’s nanotechnology. Comparing CNC to CNF, bacterial nanocellulose with
higher purity and crystallinity possess outstanding merits. The natural behavior of this nanocellulose
are high modulus, low density, has a great water holding capacity, and biocompatibility.
Nanocellulose also offers a range of exciting mechanical, optical, barrier, rheology, morphology,
degree of fibrillation, electrical and biodegradability properties. Besides, various methods of surface
modification of nanocellulose were deliberated. Surface modification pointedly improved the
nanocellulose’s tensile strength, thermal stability and thermal modulus. The most used modification
is covalently attached hydrophobic molecules to the nanocellulose hydroxyl group via acetylation,
oxidation, esterification, and sulfonation. In addition, nanocellulose is ready to have long-achieving
impacts upon numerous applications. The isolation of nanocellulose can now address business needs,
yet additionally improve the ecological issue of ozone harming substance discharged, giving
advantages in carbon sequestration and biofuel generation that will, at last, be of assistance to lessen
a worldwide temperature alteration. In blending with further distribution for subsidizing,
nanocellulose is without a doubt destined towards acquiring worldwide demand and consequently
sustaining an enormous scale generation.
Nomenclature
Abbreviations
CNC Cellulose nanocrystals MCC Microcrystalline cellulose
CNF Cellulose nanofibrils ACC Aqueous counter collision
BNC Bacterial nanocellulose ILs Ionic liquids
SEM Scanning electron
microscope HIUS
High intensity ultrasonication
TEM Transmission electron
microscope WAXS Wide-angle X-ray scattering
CAGR Compound annual growth
rate PLA Polylactic acid
TEMPO
(2,2,6,6-
Tetramethylpiperidin-
1yl)oxyl
AFM Atomic force microscopy
NaOCl Sodium hypochlorite IPTS
Isocyanatepropltriethoxysilan
e
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CAGA Compound annual growth
rate USA United States of America
PVA Polyvinyl alcohol OLED Organic light-emitting diode
LIB Li-ion battery Symbols
MWCNT Multi-walled carbon
nanotube $ United States dollar
IgG Immunoglobulin μ micro
PANI Polyaniline Å Angstrom
CTE Coefficient of thermal
expansion nm Nanometer
APS Ammonium persulfate ppm Parts per million
Acknowlegment: This work ws supported by Tenaga Nasional Berhad (TNB) and Universiti Tenaga Nasional
(UNITEN) through BOLD Refresh Publication Fund (J510050002-IC-6 BOLDREFRESH2025-Centre of
Excellence).
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