Accepted Manuscript

Title: Preparation, properties and applications of

nanocellulosic materials

Author: <ce:author id="aut0005"

author-id="S0144861716314266-
b974b492ca5375888fe5957cb55929e1"> Subrata
Mondal

PII: S0144-8617(16)31426-6
DOI: http://dx.doi.org/doi:10.1016/j.carbpol.2016.12.050
Reference: CARP 11857

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Received date: 10-4-2016

Revised date: 17-12-2016
Accepted date: 20-12-2016

Please cite this article as: & Mondal, Subrata., Preparation, properties
and applications of nanocellulosic materials.Carbohydrate Polymers
http://dx.doi.org/10.1016/j.carbpol.2016.12.050

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 Preparation, properties and applications of nanocellulosic materials

Subrata Mondal*

Department of Mechanical Engineering, National Institute of Technical Teachers’ Training and

Research (NITTTR), Salt Lake City, Kolkata, PIN 700106, West Bengal, India

* Corresponding author, S. Mondal, email : subratamondal@yahoo.com

Highlights

 Interest for the nanoscale materials derived from lignocellulosic biomass is increasing rapidly,

 Various methods of nanocellulose preparations have been reviewed,

 Methods for the surface modifications of nanocellulose have been included,

 Applications of nanocellulosic materials in various fields are discussed.

Abstract

Recently, nano materials derived from natural renewable resources have drawn much attention in

the nanotechnology research thrust. Lignocelluloses are composed of cellulosic nano-fibrils

which can be disintegrated by chemical, mechanical and enzymatic methods in order to obtain

nanocellulose. Further, nanocellulose can also be synthesized by bacterial method in a suitable

culture. Nanocelluloses have many interesting properties (viz. nano-dimension, renewability, low

1
toxicity, biocompatibility, bio-degradability, easy availability and low cost) which make them

ideal nanomaterials for diverse applications. In this paper, author reviewed researches on recent

advances in nanocellulosic materials. Various methods of nanocellulose preparation and their

properties, surface modifications of nanocellulose, and applications of nanocellulose in the

diverse fields have been discussed in the paper.

Key words: Cellulose, nanocrystal, biomedical, filler, aerogel, polymer nanocomposite.

1. Introduction

Novel materials derived from the low-cost and renewable resources has drawn significant

interests to the materials scientists with the growing environmental concern of end-of-life

disposal challenges (Abraham et al. 2011). The materials obtained from the renewable

bioresources could be the alternative of petroleum based synthetic products due to their

advantages of relatively low cost, environmental friendly in nature, easy availability,

renewability, and nontoxicity. Cellulose is the most abundant natural polymer in the planet Earth.

By photo-synthesis processes, plants synthesizes cellulose which accounts for approximately

40% of lignocellulosic biomass (Mondal, Memmott and Martin 2014, Anirudhan, Gopal and

Rejeena 2015b, Abraham et al. 2011).

Cellulosic nanofibrils are mainly composed of plant cell walls and provide strength, toughness

and stiffness to the plant anatomy. Cellulosic nanofibrils in the form of nanocellulose can be

extracted from the lignocellulosic bioresources by using appropriate chemical, mechanical,

enzymatic or combination of more than one method. Nanocellulosic material has been attracted

considerable research attention in recent years (Figure 1) due its many exceptional properties and

2
potential for the diverse applications (Donius et al. 2014). Nanobiomaterials derived from

abundant and renewable natural resources could have the potential to replace synthetic

nanomaterials (Deepa et al. 2015). Nanocellulosic materials have many interesting features such

as nano dimension (higher surface area to volume ratio), nontoxicity, biodegradability,

biocompatibility etc. Interesting properties of nanocellulose could find applications in the

biomedical field, reinforcement in polymer matrix in order to fabricate nanocomposite, energy,

environment and so on so forth.

By definition, material that has at least one dimension less than or equal to 100 nm, could be

considered as nanomaterial (Espino-Perez et al. 2014). Nanomaterials derived from renewable

cellulosic and lignocellulosic biomass could play a significant role in the nanotechnology

research domain (Gardner et al. 2008, Milanez et al. 2013, Milanez et al. 2014). Owing to the

hierarchical structure of cellulose molecules in the lignocellulosic biomass, nanocellulose can be

extracted by using an appropriate extraction methods (Dufresne 2013). Various types of plant

biomasses can be used to extract nanosized cellulose, and the yield of nanocellulose could

depends on the source of lignocellulosic biomass, when same method of extraction would be

employed (Deepa et al. 2015). Advances of nanotechnology research encourage scientists to

develop nanomaterials from renewable bio-resources which have significantly lowered

environmental impact. Therefore, in this review paper, author attempted to review the extraction

of nanocellulose from various lignocellulosic biomasses, surface modification of nanocellulose,

the characterization of nanocellulose and their potential applications in the diverse fields.

2. Various methods for the preparation of nanocellulosic materials

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Nanocelluloses are accounted for various types of cellulosic nanomaterials with at least one of its

dimensions is less than or equal to 100 nm by the definition of nanomaterials. Typical examples

of nanocelluloses are cellulose nanofibrils (CNFs), cellulose nanocrystals (CNCs) and bacterial

nanocellulose (BNC) (Aitomaki and Oksman 2014, Charreau, Foresti and Vazquez 2013, Jorfi

and Foster 2015, Plackett et al. 2014, Lin and Dufresne 2014). Nanocellulose can be extracted

from various lingocellulosic plant resources (Chen et al. 2015a, Chen et al. 2015b) by using

mechanical, chemical or enzymatic methods. Lignocellulosic biomass is a complex biomaterials

which consists of cellulose, hemicellulose, and lignin. Cellulose in the lignocellulosic biomass

can be disintegrated to nano dimension materials by using appropriate methods (Lee, Hamid and

Zain 2014a). Macro or micro structure of cellulose consists of amorphous as well as crystalline

phases. It is relatively easy to break the amorphous phase of cellulosic biopolymer by

mechanical, chemical or enzymatic means, while, it is quite difficult to break the nanostructured

crystalline phase of cellulose due to the presence of enormous hydrogen bonding. Extraction of

nanocellulose from the cellulosic biomass includes two major steps viz. pretreatment and

removal of amorphous phase by appropriate methods (Kim et al. 2015). Prior to the mechanical,

chemical treatment or enzymatic treatment, pretreatments such as alkali treatment and bleaching

are required. The prime objective of pretreatment is to remove certain amount of lignin,

hemicellulose, wax and oils which cover on the external surface of the fibre cell wall. Alkali

treatment depolymerises the native cellulose structure, defibrillates the external cellulose

microfibrils and exposes short length crystallites. Further, bleaching treatment is required in

order to remove the cementing material completely from the fiber (Abraham et al. 2011). Nano

dimensions, quality and yield of nanocellulose would depend on source of lignicellulosic

biomass when same method of extraction is applied. Abraham et al. reported nanocellulosic

4
materials extracted from three different lignocellulosic biomasses such as banana (pseudo stem),

jute (stem) and pineapple leaf fibre by pretreatment with alkali followed by steam explosion and

finally acid hydrolysis. The quality and yields of nanocellulose derived from pineapple biomass

is better than the nanocellulose extracted from banana and jute stem (Abraham et al. 2011).

Apart from cellulose nanocrystal and cellulose nanofibers, nano size bacterial nanocellulose

(BNC) can be synthesized by certain strains of bacteria in a favorable condition (Aitomaki and

Oksman 2014).

2.1. Mechanical methods

Nanocellulose can be obtained by disintegrating cellulose from the lignocellulosic biomass by

mechanical means (Hettrich et al. 2014). Cherian et al. reported acid coupled steam treatment

method for the preparation of nanocellulose from pineapple leaf fiber (Cherian et al. 2010). The

surface morphology of biomass changes with the removal of primary components (Figure 2).

Pretreatment of biomass at high temperature steam explosion with alkali hydrolyzes

hemicellulose and depolymerizes the lignin. Further, lignin is rapidly oxidized by chlorine and

accelerate the degradation of lignin. Formation of various groups such as hydroxyl, carbonyl and

carboxylic groups facilitates the lignin solubilization in the alkaline medium. Acid coupled steam

treatment helps to disintegrate fibrils to form the nanocellulose (Cherian et al. 2010). Hettrich et

al. reported a combined chemical and mechanical method for the preparation nanocellulose by

using various cellulosic bioresources such as bleached pulp, cotton linters and microcrystalline

cellulose. Prior to the mechanical treatment, pretreatments such as grinding, acid hydrolysis,

decrystallization and derivatization are used for the preparation of nanocellulosic materials.

Extracted cellulose has spherical shape with diameter of less than 200 nm (Hettrich et al. 2014).

Jiang and Hsieh reported a method for the cellulose nanofibrils preparation by using mechanical

5
defibrillation of rice straw using a high speed blender in three consecutive blending and

separation steps (Jiang and Hsieh 2013). Nanocellulose can be derived from the lingocellulosic

biomass by high pressure homogenization. The biomass could be suspended by high speed

stirring coupled with ultrasonication treatment prior to the high pressure homogenization (Wang

et al. 2015a). Ionic liquid can be used to treat the lignocellulosic biomass prior to the mechanical

treatment. The ionic liquid permeates through the microstructure of cellulose and subsequently,

attacks the hydrogen bonds between cellulose molecules. During high pressure homogenization,

inter and intra molecular bonds are further destroyed, hence, nanocellulose is disintegrate from

the biomass. Extracted nanocellulose has a width of 10-20 nm (Li et al. 2012, Wang et al.

2015b).

2.2. Chemical method

Acid hydrolysis is a common method to extract nanocelluose from the lignocellulosic biomass

(Lin, Bruzzese and Dufresne 2012a, Lu et al. 2013, Saraiva Morais et al. 2013, Yongvanich

2015, Moran et al. 2008, Mandal and Chakrabarty 2011). After the hemicellulose removal and

prior to the acid hydrolysis treatment, the lignocellulosic biomass can be treated with chemical

such as dimethyl sulfoxide to swell the matrix of biomass so that acid could diffuse into the

domain structure of lignocellulosic biomass easily and disintegrate the nanowhisker (Mandal and

Chakrabarty 2011). In an acid treatment method, yield of nanocellulose depends on the content

of lignocellulosic biomass and the reaction conditions such as acid concentration, time and

temperature. Optimization of experimental parameters are required to obtain maximum yield and

to preserve the nanocellulose morphology (Lu et al. 2013). Yield as well as nano dimension of

6
nanocellulose decreases with the increase of acid treatment time of cellulosic biomass (Shahabi-

Ghahafarrokhi et al. 2015). Preparation of nanocellulose from the lignocellulosic biomass by

using catalysts could be a green approach. Ionic liquid based catalyst has several advantages viz.

wide range of electrochemical stability, good electrical conductivity, high ionic mobility,

selective dissolution properties to many organic and inorganic substances as well as excellent

chemical and thermal stabilities (Abd Hamid, Al Amin and Ali 2014). Ultrasound has significant

influence on nanocellulose property prepared from bleached hardwood kraft pulp oxidized by

2,2,6,6- tetramethylpiperidine-1-oxyl (TEMPO). Nanocellulose prepared by using ultrasound

assisted process is thinner, contain more carboxylic functionality, higher degree of fibrillation,

and higher yield (Mishra et al. 2012, Mishra et al. 2011, Mueller et al. 2013, Loranger et al.

2012). Satyamurthy and Vigneshwaran proposed a novel method of nanocellulose preparation in

an anaerobic microbial consortium for the controlled hydrolysis of microcrystalline cellulose

which was obtained from cotton fibers. The advantages of this method are less energy

consumption due to enzyme (cellulase) assisted catalysis, no surface sulfation, preserve the

chemical structure of cellulose, biocompatible as well as potential to scale up (Satyamurthy and

Vigneshwaran 2013).

2.3. Bacterial method

Nanocellulose obtained by using bacterial method has similar chemical structure as with

nanocellulose extracted from the lignocellulosic biomass by following chemical and mechanical

methods. In addition to this, ultrafine nanofiber network formed by an appropriate culture

medium exhibits unique properties e.g. high purity, uniform morphology, good water absorption

7
capacity, excellent mechanical properties and flexibility (Taokaew et al. 2013, Iguchi, Yamanaka

and Budhiono 2000, Chen et al. 2009). Biomaterial grade bacterial nanocellulose (BNC) could

be synthesized by aerobic cultivation of the bacterium Gluconacetobacter xylinus (synonym

Komagataeibacter xylinus) in a glucose enriched medium (Ahrem et al. 2014, Gatenholm and

Klemm 2010, Feldmann et al. 2013, Fu et al. 2013, Kubiak et al. 2014). Aramwit and Bange

reported method of bacterial nanocellulose preparation by using the coconut water at suitable

culture media by a gram negative rod shaped bacterium, G. xylinus (Aramwit and Bang 2014).

3. Properties of nanocellulose

Morphological structure of nanocellouse is highly dependent on the efficient removal of non

cellulosic part and dissolution of amorphous region of domain structure (Cherian et al. 2010, Lu

et al. 2013). Morphology (Table 1), physical property and dimension of the nanocelluloses are

varied significantly with the different natural fiber resources and with the extraction processes.

Deepa et al reported the morphology of nanocelluloses which were extracted by acid hydrolysis

from sisal, pineapple leaf and coir; the nanofiber shows long, flexible and entangled morphology,

whereas, more individualized and rod like structures (Figure 3) are visible when nanocellulose is

extracted from the banana rachis and kapok (Deepa et al. 2015).

Mechanical properties of the nanocellulose are better than their lingocellulosic source biomass

materials because of more uniform morphological structure. The average modulus of

nanocellulose is 100 GPa which is much higher than the base celluloseic materials (Dufresne

2013). Crystal structure and degree of crystallinity of the nanocellulose depends on the

lignocellulosic resources (Le Bras, Stromme and Mihranyan 2015). Nnanocellulose contain both

8
cellulose I and cellulose II, which could be characterized by typical X-ray diffraction peaks at

around 2(θ) ~23° and 2(theta)~34° respectively (Peng et al. 2013).

Thermal degradation property of nanocellulose depends on extraction procedure and source of

cellulose bio-resources. In general, nanocellulose obtained from extracting natural cellulosic

resources have better thermal stability than the α-cellulose present in the original lignocellulosic

biomass (Abraham et al. 2011). Improved thermal stability of nanocellulosic materials as

compared to their source cellulose is due to their higher crystallinity, flexible structure and

removal of low thermal stable lignin materials (Deepa et al. 2015).

Carboxylic functional group (189 – 1181 mmol/kg) containing nanocellulose gel shows shear

thinning rheological behaviors. Therefore, with the increase of shear rate, nanocellulosic gel

network slowly broke up into individual entities, hence, reduces the final viscosity of the gels

(Loranger et al. 2012, Loranger et al. 2013). Surface property of the nanocellulose would affect

the shear thinning rheology of the suspension (Rees et al. 2015).

4. Surface modification of nanocellulose

Bulk applications of nanocellulose are often hindered due to the poor dispersibility of

nanocellulose in nonpolar organic solvent, and nonpolar polymer matrix (in order to prepare the

nanocomposite) (Kovalenko and Iop 2014). Cellulosic nanofiller has a tendency to aggregate due

to the inter and intra molecular hydrogen bonding between three hydroxyl groups of the repeat

unit, and this results in poor dispersion of nanofillers in non polar solvent and non polar polymer

matrices. In order to utilize the nanofillers properly, the fillers should be homogeneously

dispersed and distribute in the matrices. Nanoscale dimension of nanocellulose has high specific

9
surface area which ensures plenty of hydroxyl groups on the nanocellulose surfaces which could

be used for the chemical modification of nanocellulose surface (Lin, Huang and Dufresne

2012b). Chemical modification should be mild to preserve the other useful properties of

nanocellulose. Chemical modification of nanocellulose can be classified into three groups a)

molecules grafting on nanocellulose, b) molecules grafting to nanocellulose, b) substitution of

hydroxyl groups with small molecules (Dufresne 2013). Various strategies of nanocellulose

modifications are illustrated schematically in Figure 4.

Espino-Perez et al. proposed solvent free chemical modification of nanocellulose with carboxylic

groups. Appropriate functional molecules could be attached with nanocellulose by SolReact

method by esterification of hydroxyl groups of nanocellulose with carboxylic groups of aromatic

carboxylic acids. The method has several advantages such as less toxic carboxylic acid for

grafting, low reaction temperature, reaction at ambient pressure and recycle of excess reactant by

distillation technique (Espino-Perez et al. 2014). Carboxylic functionalities could introduce into

the nanacellulose by oxidation method, and the carboxylic functionalities could serve as

templates to bind various biomolecules such as fluorescent amino acids, peptides etc. Amino

acid or peptide can bind with oxidized nanocellulose by nucleophilic reaction between the amine

group (-NH2) and carboxylic group (Barazzouk and Daneault 2011, Barazzouk and Daneault

2012a, Barazzouk and Daneault 2012b). In general, carboxylic functionalities are introduced into

the nanocellulose surfaces by carboxymethylation or 2,2,6,6- tetramethylpiperidine-1-oxyl

(TEMPO) mediated oxidation method (Carlsson et al. 2014).

Surface chemistry of nanocellulose can be engineered by pretreatment of the raw nanocellulose

fibres by using carboxymethylation and periodate oxidation methods. Pretreatment introduces

aldehyde and carboxyl groups on the nanocellulose surface. Further, aldehyde and carboxylic

10
functionalities could react with other appropriate functional groups to form covalent bonding, for

an example, aldehyde can react with amine to form covalent bonding of polymer-protein

conjugation (Chinga-Carrasco and Syverud 2014). Poor suspension of nanocellulose in aqueous

media can be improved by grafting of acrylamide on nanocellulose surface by redox inititation

grafting method. The nanocellulose grafted with acrylamide shows self assembly of lyotropic

state (Yang and Ye 2012). Hydroxyl groups of nanocellulose can be oxidized to dialdehyde by

NaIO4 at appropriate experimental condition (Lu et al. 2014). Surface of the nanocellulose can be

modified by phosphorylation technique with phosphoric acid as negatively charged phosphoryl

donor (Kokol et al. 2015).

Dispersion and distribution of nanocellulose in the polymer matrix can be improved by surface

modification of nanocellulose with appropriate molecules. In order to impart hydrophobicity to

the nanocellulose, a long hydrophobic alkyl chain can be substituted from the hydroxyl

functionality of nanocellulose via bimolecular nucleophilic substitution (Bae and Kim 2015).

Benkaddour et al. proposed surface modification of oxidized nanocellulose with long chain

polycaprolactone diol (PCL) using click chemistry and esterification reaction. Higher grafting

yield can be observed with click chemistry as compared with the esterification reaction. PCL

grafted nanocellulose with improved hydrophobicity could be suitable for the reinforcement in

the hydrophobic polymers (Benkaddour et al. 2013). Bacterial nanocelluose can be modified

with xyloglucan (XG) and xyloglucan bearing a GRGDS pentapeptide to improve the wettability

and cell adhesion. Modified bacterial nanocellulose could be a potential candidate of new

biomaterial (Bodin et al. 2007).

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5. Application of nanocellulosic materials

5.1 Biomedical applications

Scaffolds that could be prepared by using bacterial nanocellulose (BNC) is ideal for many

biomedical applications due to their unique characteristics such as high porosity, excellent wet

mechanical properties, noncytotoxicty, and biocompatibility (Hong, Wei and Chen 2015, Innala

et al. 2014, Kramer et al. 2006, Krontiras, Gatenholm and Hagg 2015, Kuzmenko et al. 2013,

Sundberg, Gotherstrom and Gatenholm 2015, Nimeskern et al. 2013, Park, Lee and Hyun 2015,

Pretzel et al. 2013, Taokaew et al. 2013, Moritz et al. 2014, Mueller et al. 2014a, Martinez Avila

et al. 2015). 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidized nanocellulose film exhibits

excellent cell adhesion and proliferation to be used as a potential candidate for the development

of biomaterials (Hua et al. 2014, Park et al. 2015, Zander et al. 2014). Further, TEMPO oxidized

bacterial nanocellulose can be used to prepare the hydrogel with elastin likes polypeptide (ELP).

Positively charged ELP would behave like a polymeric crosslinker with negatively charged

nanocellulose. Hybrid hydrogel has properties like noncytotoxicity and capability to encapsulate

cells that could find the potential applications in the biomedical fields (Cheng, Park and Hyun

2014).

Chinga-Carrasco and Syverud reported pH sensitive nanocellulose hydrogel which could be

prepared from the surface functionalized wood nanocellulose (Chinga-Carrasco and Syverud

2014). Bacterial nanocellulose scaffold with excellent porous architecture has good mechanical

properties, maintain a structural integrity, excellent biocompatibility, supports cell in growth, and

secures tissue integration could be used for the auricular cartilage reconstruction (Avila et al.

2014, Martinez Avila et al. 2015, Martinez Avila et al. 2014). Avila et al. reported bacterial

12
nanocellulose and alginate biphasic porous scaffold for the auricular cartilage reconstruction

(Avila et al. 2015). Bacterial biosynthesized nanocellulosic hydrogel in static mode shows an

extracellular, highly crystalline cellulose molecules, and a flat shaped hydrogels at the surface of

the culture medium. The structure formed by irregular alignment of the BNC nanofibers is

similar to those of collagen matrices. However, small and heterogeneous pore size of scaffold

limits its use as implant material for the tissue engineering due the difficulty in growth of cells.

Laser patterning could make scaffold favorable to support cell in growth for the cartilage

remodeling for the joint (Ahrem et al. 2014). Bacterial nanocellulose construct has excellent

properties such as tissue regeneration, faster healing properties, shape stability, controlled drug

delivery etc. and all these required for large skin transplantation, wound dressing and

reconstructive surgery (Fu et al. 2013, Moritz et al. 2014, Mueller et al. 2014b). The favorable

biomedical property of bacterial nanocellulose and the conductive property of polypyrrol could

tailored the nanocomposite for the tissue engineering which require electrical conductivity such

as nerve tissue reconstruction (Muller et al. 2013).

Apart from the kidney transplantation, haemodialysis remains other treatment method for the

patients with chronic renal failure. Polymer nanocomposite membrane could be prepared with

conductive polypyrrole and nanocellulose for haemodialysis membranes. The nanocomposites

membrane could combine the active ion exchange and passive ultrafiltration with the large

surface area (Ferraz et al. 2012a, Ferraz et al. 2013, Ferraz and Mihranyan 2014, Ferraz et al.

2012b). Further, nanocellulose-polypyrrole composite membrane could be an excellent candidate

for the applications in electrochemically controlled extraction and separation of biologically

interesting compounds (Nystrom et al. 2010). Razaq et al. proposed highly porous polypyrrol-

nanocellulose composite ion exchange membrane for the solid phase extraction of biomolecules

13
by reversible electrochemically controlled process. Polypyrrol layer in the composite membrane

ensured excellent access to the ion exchange molecules (Razaq et al. 2011).

Microporous cellulosic hydrogel has the capability to functionalized biomolecules and could find

potential application for the wound healing. Nanocellulosic hydrogel with smart pH responsive

property for biosensing can manage chronic wounds for controlled and intelligent release of

antibacterial components (Chinga-Carrasco and Syverud 2014). Ultrafine and extremely pure

fibrous network structure of silk sericin releasing bacterial nanocellulose gel prepared at an

appropriate culture media could find applications in facial treatment. Silk sericin has many

interesting properties for biomedical applications such as biocompatibility, antioxidant,

bioadhesive, and bioactive activities. Further, the biomaterial shows excellent mechanical

properties comparable to that of the commercial paper mask, biodegradability, less adhesive than

paper mask (therefore, can be easily removable without pain) and noncytotoxic (Aramwit and

Bang 2014). Nanocellulose based modified superabsorbent polymer composite could be used as

biomedical application for drug delivery unit (Anirudhan and Rejeena 2014, Lin et al. 2012a).

Shape memory aerogel with an excellent water absorption (due to the presence of numerous

surface polar group viz. hydroxyl and carboxylic groups) capacity can be prepared by using the

modified nanocellulose in a freeze drying method. The aerogel retain excellent physical integrity

in water, while, demonstrating full and repetitive shape recovery with repeated cycles required

for biomedical applications (Jiang and Hsieh 2014). Nanocomposite prepared by modified

nanocellulose and collagen could be used for the tissue engineering scaffold due its excellent

biomedical properties such as biocompatibility, cell adhesion and proliferation (Lu et al. 2014).

Other applications of nanocellulose in the biomedical field includes, silver nanoparticle

containing porous three dimensional network structure of bacterial nanocellulose construct could

14
find the applications for the antimicrobial wound dressings. Silver nano-particle can be

immobilized by chemical linkage on porous nanocellulose network which can prevent the release

of nano particles from the network structure (Berndt et al. 2013). Antibacterial property of

nanocellulose could be improved by allicin and lysozyme. Allicin and lysozyme conjugated

nanocellulose possesses a good antifungal as well as antibacterial effects, which could be useful

to prepare antibacterial fabrics for the medical textile applications (Jafary et al. 2015, Jebali et al.

2013). Favorable surface chemistry, morphology, rheology and ability to inhibit bacterial growth

are useful characteristics of nanocellulose required for the bio ink in 3D printing of porous

wound dressing material for potential to carry and release antimicrobial components (Rees et al.

2015). Bio ink based on nanocellulose and aliginate for the potential use of bio printing of

biomaterials is proposed by Markstedt et al. The developed bio ink is able to print both 2D and 3

D construct of shaped cartilage structures (Figure 5), such as a human ear and sheep meniscus

etc. (Markstedt et al. 2015). As a coordinated process, bone regeneration is mainly regulated by

multiple growth factors. Nanocellulose (NC) based biphasic calcium phosphate with 0.5% NC

loading scaffold shows that the growth factors were released from NC in a sustainable manner

for the required period. Biphasic scaffold showed higher cell attachment and proliferation

behavior which could be beneficial for improved bone regeneration (Sukul et al. 2015).

Nanocellulosic hydrogel scaffold, containing both osteoconductive and osteoinductive properties

which could enhance bone regeneration. Slower degradation rate of the scaffold is due to the

presence of nanofibrillar cellulose, and the slower degradation rate favored the sustainable

release of simvastatin (an osteoinductive molecule) to enhance osteogenesis (Sukul et al. 2015a).

5.2 Energy, environmental and water related applications

15
Nanocellulose and conductive electro-active composite material retain both constituent’s unique

responsive properties viz. nanocellulose as a matrix provide flexibility, whereas electroactive

material provide electrical properties. The developed composite material has potential

applications for the flexible electrodes, flexible display, biocompatible energy scavenging, and

so on (Shi, Phillips and Yang 2013). Aerogel based on nanocellulose with the high surface area

and surface charge can be used for the layer-by-layer assembly on conductive polymer, carbon

nanotube, titanium dioxide, zinc oxide, aluminum oxide to enhance the charge capacity,

flexibility and mechanical properties for the application in energy storage and other electronic

applications (Hamedi et al. 2013, Korhonen et al. 2011a). Conducting composites based on

polypyrrol and nanocellulose could be applicable in environmentally friendly energy storage

devices with commercially viable mass loadings, capacitances, and energy densities (Figure 6)

(Carlsson et al. 2013, Tammela et al. 2015, Wang et al. 2015c, Wang et al. 2015d, Wang et al.

2014b, Zhang et al. 2013, Mihranyan et al. 2012). Nanocellulose can be used to prepare the

rechargeable power sources based on unitized separator/electrode assembly (SEA) construct.

Paper batteries based on electrode made with cellulose nanofibrils (CNF)/multiwalled carbon

nanotubes (MWNTs) demonstrated ultra thin (hence, high-mass loading) electrodes far beyond

those accessible with conventional battery technologies. Ultrathin electrode in combination with

readily deformable CNF separators allows fabrication of user friendly paper batteries via origami

folding techniques (Cho et al. 2015). The cellulose nanofiber paper-derived separator membrane

is an electrolyte-phillic, nanoscale labyrinth structure formed by closely packed CNFs. The

cellulose nanofiber paper separator prepared with appropriate experimental condition contained

highly interconnected nanoporous network channels with good mechanical properties, excellent

separator properties with improved cell performance (Chun et al. 2012). The CNF separator tightly

16
secure the interlocked electrode–separator interface. The unique physico-chemical structure of

the SEAs drastically improves the mass loading of electrode active materials, electron transport

pathways, electrolyte accessibility etc. (Choi et al. 2014). Further, incorporation of silica (SiO2)

nanoparticles allows loose packing of CNFs as a result of more porous structure which allows

better ionic conduction due to the tailored combination of nanoporous structure and separator

thickness, and all these properties contributed to the excellent cell performance of the separator

membrane (Kim et al. 2013).

Kang et al. reported an all-solid-state flexible supercapacitors of bacterial nanocellulose, carbon

nanotubes and ionic liquid based polymer gel electrolytes with high physical flexibility, desirable

electrochemical properties, excellent cyclability and superior mechanical properties (Kang et al. 2012).

Mechanically strong and highly conducting composite of nanocellulose and carbon nanotube can

be prepared from the aqueous dispersion in the form of semitransparent conductive films,

aerogels and anisotropic microscale fibers. Excellent colloidal stability of aqueous dispersion

provided simple and cost effective method for self assembly of advanced hybrid nanocomposites

for energy applications (Hamedi et al. 2014, Henry et al. 2015).

Nanocellulose based paper possesses superior optical clarity as compared with the regular paper

substrate. Transparent and conductive paper can be prepared by deposition of titanium oxide,

carbon nanotube, silver nano-rod, tin-doped indium oxide, boron nitride, silica nanoparticles,

quantum dot and molybdenum disulfide on nanocellulosic paper substrate. Transparent

conductive paper could find potential applications in wide range of optoelectronics viz. displays,

touch screens and interactive paper, organic solar cell, lithium ion battery, energy storage devices

and so on (Hu et al. 2013, Li et al. 2015b, Liu, Sui and Bhattacharyya 2014, Uetani, Okada and

17
Oyama 2015, Wang et al. 2015e, Xue et al. 2015). Composite based on nanocellulose and

polypyrrole is a promising material for electronic applications due to its large surface area and

capability to store charges. Polypyrrole nanocellulosic composite paper based energy storage

device has several advantages such as high cell capacitances, superior rate capabilities, excellent

cycling performances, high performance, light weight and low cost (Kizling et al. 2015, Nystrom

et al. 2010, Razaq et al. 2012, Wang et al. 2014c). Nanocomposite paper based on nanocellulose

with surface carboxylic groups and carbon nanotube has good mechanical properties, flexibile,

excellent electrical conductivity, inexpensive and environmental friendly, and could find

potential for a wide range of flexible electronics (Koga et al. 2013).

Ecofriendly, flexible and electrically conductive nanocomposite of nanocellulose and polyaniline

can be prepared by in-situ polymerization for the applications of flexible electronic, antistatic

coatings, and electrical conductors (Liu et al. 2014, Nguyen Dang et al. 2013). Wang et al.

proposed a novel method of carbon aerogel anode preparation for the lithium battery. Carbon

aerogel with large open pores and high surface area can be prepared by pyrolysis of three

dimensional bacterial nanocellulosic hydrogel construct. Carbon aerogel shows very good

electrochemical performance in terms of both capacity retention and rate performance required

for the lithium ion batteries (Wang et al. 2014a). Kobayashi et al. proposed a three dimensional

aerogel prepared by acid induced gelation and super critical drying of liquid crystalline

nanocellulose which is extracted from wood cellulosic biomass. The aerogel with high porosity,

large internal surface area, good mechanical and heat insulation properties could be used as

thermal, acoustic, or electrical insulators (Kobayashi, Saito and Isogai 2014). Properties of

nanocellulose such as degree of crystallinity and water sorption capacity may have significant

influence on the dielectric properties of nanocellulosic composite materials for electrical

18
insulator applications (Le Bras et al. 2015). Kaoline and nanocellulose composite could be

promising for the cost effective, flexible, low surface roughness and porosity substrate for

printed electronic applications (Penttila et al. 2013, Torvinen et al. 2012).

Jiang et al. proposed a Nafion and bacterial nanocellulose composite membrane for the proton

exchange membrane fuel cell (PEMFC) and direct methanol fuel cell (DMFC). Annealing of

composite membrane significantly decreases the water uptake, volume swelling ratio and

methanol permeability, due to the increased dense structure, while, increases the Young’s

modulus and selectivity (Jiang et al. 2015a).

Nanocellulose based adsorbent has the potential to effectively remove toxic components from the

aqueous waste water (Anirudhan and Shainy 2015, Anirudhan, Deepa and Binusreejayan 2015a,

Arsad and Ngadi 2014, Hokkanen, Repo and Sillanpaa 2013, Kardam et al. 2014). Anirudhan et

al. reported a composite adsorbent based on poly(itaconicacid)- poly(methacrylicacid)-grafted

nanocellulose/nanobentonite for the removal of Uranium from the aqueous solution. Adsorption

capacity of resultant adsorbents increases with increasing carboxylic group concentration on the

surface of adsorbents. Further, high surface area enhanced the adsorption capacity of adsorbents

(Anirudhan et al. 2015a). Suman et al. proposed a composite adsorbent based on nanocellulose –

silver nanoparticles embedded pebbles for the cost effective and reusable system for effective

removal of contaminants such as dyes, heavy metals and microbes from the aqueous media. In

the composite adsorbent, silver nano-embedded pebbles remove or kill microbes, whereas,

nanocellulose remove the dyes and heavy metal (Suman et al. 2015).

The photocatalytically active and stable hybrid materials of bacterial nanocellulos and TiO2 can

be used for the purification of water and polluted air (Wesarg et al. 2012). Zhang et al. reported

19
an ultra light, flexible, hydrophobic as well as oleophillic sponge based on nanocellulose and

methyltrimethoxysilane sols which could be prepared by freeze drying. The spongy adsorbents

can adsorb a wide range of toxic organic solvents and oils with capacities up to 100 times of its

own weight, depending on the solvent and oil properties (Figure 7). Silylated nanocellulose

sponges has excellent flexibility, and shape stability in oil and solvent (Zhang et al. 2014).

Carbon aerogel could be prepared by controlled pyrolysis of nanocellulose hydrogel construct.

Aerogel exhibits excellent oil adsorption capacity due to its micro porous network structure, high

surface area, ultra light density with hydrophobic property (Meng et al. 2015). The surface

modified aerogel with the silanes could be useful for the separation of oil from the aqueous

solution of water and oil. Modified aerogel material has light weight and hydrophobic in nature,

therefore, float on water surface at the same time absorb oil in order to separate oil from the

aqueous solution. The adsorbents could adsorbed oil few times on its own weight and adsorbed

oil can be recovered, hence, the adsorbents are reusable (Cervin et al. 2012). Incorporation of

nanoparticles into the nanocellulose substrate produce novel nanocomposite which could be used

as potential detector to detect trace contaminants in aqueous solution. For an example, bacterial

nanocellulose and gold nanoparticle composite based detectors have light weight, flexible, shape

stable in aqueous acidic and alkalinie solution (Wei et al. 2015, Wei et al. 2014).

Hydrophilic characteristic of nanocellulose is useful for the preparation of hydrogel adsorbent.

However, enormous hydroxyl groups on the adsorbent surface cause aggregation, hence, limits

its application as adsorbents, and this could be improved by surface modification of adsobents

with selective molecules (Anirudhan and Shainy 2015). Modified nanocellulose based

adsorbents with high surface area and engineered surface functionalities could be used to recover

useful biomolecules such as beta-Casein, trypsin, lysozyme, immunoglobulin, hemoglobin,

20
hemoglobin, from the aqueous solution (Anirudhan et al. 2015b, Anirudhan and Rejeena 2012a,

Anirudhan and Rejeena 2012b, Anirudhan and Rejeena 2013a, Anirudhan and Rejeena 2013b,

Anirudhan, Rejeena and Tharun 2013). Nanocellulose has plenty of surface functional groups

such as hydroxyl groups which could be functionalized with appropriate molecules for the

selective removal of toxic biomolecules such as Fumonisin B1, aflatoxin B1, humic acid etc.

from the aqueous solution (Jebali et al. 2015a, Jebali et al. 2015b, Jebali et al. 2015c).

Highly porous, free standing, and light weight sponge like nanocellulosic aerogel can be

prepared by freeze drying of aqueous suspension of nanocellulose. The surface morphology such

as porosity and surface area of aerogel can be controlled by nanocellulose quality and

concentration in the suspension (Chen et al. 2014). The TiO2-coated nanocellulose aerogels with

photocatalytic activity is very useful for the water purification applications (Kettunen et al.

2011). Titanium dioxide coated nanocellulose aerogel has oleophilic property, low density and

high adsorption capacity to adsorb organic contaminant from the wastewater surface (Korhonen

et al. 2011b). Filter paper can be prepared by highly crystalline nanocellulose. The filter paper

with tailored pore size distribution could be particularly suitable for the removal of virus

(Metreveli et al. 2014). Various polystyrene latex bead sizes of 500, 100, and 30 nm

(representing the virus size) (Figure 8) are filtered out by the porous crystalline nanocellulosic

filter paper.

5.3 Polymer nanocellulose composite

Nanocellulose could be an excellent environmental friendly nanofillers for the reinforcement in

the polymer matrix in order to prepare nanocomposite due to its nontoxicity, biodegradability,

21
low density, excellent mechanical properties and nanosize dimension with higher surface area,

hence, a huge interface with the matrix polymers (Abraham et al. 2012, Abraham et al. 2013,

Aitomaki and Oksman 2014, Ching et al. 2015, Costa et al. 2014, Juntaro et al. 2007, Li,

Mascheroni and Piergiovanni 2015a, Khan et al. 2014, Khan et al. 2010, Kose et al. 2011,

Kuzina et al. 2013, Qua and Hornsby 2011, Saxena et al. 2012, Zhou et al. 2012, Lani et al.

2014, Lee et al. 2014b, Lee et al. 2009, Li et al. 2014, Li et al. 2013, Li, Renneckar and Barone

2010, Pereda et al. 2011, Reddy and Rhim 2014, Tome et al. 2013, Voronova et al. 2012). One of

the major challenges for the reinforcement of natural fillers e.g. nanocellulose in the polymer

matrix is the incompatibility between polar (due to extensive surface functional groups)

nanocellulosic fillers and nonpolar polymer matrix. Enormous hydroxyl groups on the cellulose

nanocrystals (CNCs) limit their dispesibility in the hydrophobic polymer matrix. Gwon et al.

modified the CNCs using toluene diisocyanate (TDI) to overcome the poor of dispersibility in

the poly(lactic) acid (PLA) matrix. TDI-modified CNCs (mCNCs) shows good dispersion in the

PLA matrix with improved interfacial interaction between the nanofillers and polymer matrix,

when nanocomposites were prepared by solvent casting (Gwon et al. 2016). Crystallinity of the

PLA-CNC nano-composites increases with increasing CNC content in the nano-composites

which were prepared by melt compounding and melt fiber spinning followed by compression

molding, indicating that CNC can act as nucleating agent in crystallization process. In addition,

incorporation of CNC increases storage modulus of the PLA film and influences the glass

transition temperature (Sullivan et al. 2015).

Hervy et al. proposed a green composite prepared by using bacterial cellulose (BC) and

nanofibrillated cellulose (NFC) as reinforcement in epoxy matrix to prepare environmental

friendly nanocomposites. The environmental impact of the nanocomposites were evaluated using

22
life cycle assessment (LCA). Nanocellulose-reinforced epoxy composites with high

nanocellulose loading is desirable to produce nanocomposite materials with “greener credentials”

(Hervy et al. 2015).

Juntaro et al. modified the sisal and hemp fiber by bacterial nanocellulose to be used as filler for

the preparation of green composite based on cellulose acetate butyrate (CAB) and poly-L-lactic

acid (PLLA) as a matrix. Nanocellulose modified fiber shows better adhesion in the polymer

domain structure, hence, subsequently improves the mechanical properties of composites

(Juntaro et al. 2007). Nanocellulose reinforced polymer composite could be useful as ecofriendly

materials for packaging, agriculture, membrane as well as in hygienic devices. Nanocellulose can

be used to modify the natural fiber to improve the the mechanical and interfacial properties by

filling the stria and increasing the bonding with interfibrils of natural fiber (Dai and Fan 2013).

Reinforcement of nanocellulosic filler into the noncrosslinked and crosslinked natural rubber

significantly improves the mechanical properties, and increases the degradation rate as compared

with the original natural rubber. As expected, noncrosslinked natural rubber degrades at faster

rate as compared with its crosslinked counterpart. Three dimensional network structure of the

crosslinked rubber entraped the nanofillers, which subsequently restrict the degradation of the

composite materials (Abraham et al. 2012). Aerogel prepared from soya protein is brittle, and

limits its potential applications. The mechanical properties of soya protein aerogel could be

improved by reinforcement of nanocellulose. Nanocellulosic composite aerogel has high surface

area, low density and good mechanical properties, and all these improved properties make

composite aerogel an useful candidates for potential applications in packaging, thermal and

acoustic insulation, transport media, etc (Arboleda et al. 2013). Shape memory materials have

the capability of fixing a temporary shape and recover to the original shape by the applications of

23
external stimuli. Shape memory polymers have many advantages as compared with other shape

memory materials (viz. ceramic, metal alloy etc.), such as low cost, light weight, storable large

deformation etc. Some of the polymers such as segmented polyurethane shows shape memory

properties. However, segmented polyurethane has low stiffness as compared with the shape

memory ceramic and metal alloy. The mechanical properties of shape memory polyurethane can

be improved by reinforcement of nanocellulose in the polyurethane domain structure (Auad et al.

2008, Auad et al. 2012).

Due to its nontoxic in nature, packaging materials based on nanocellulose composite have great

potential to enhanced quality, safety, and stability of packaged foods (Khan et al. 2014).

Nontoxic and biodegradable biopolymer such as starch and chitosan could be used to elaborate

edible films or coatings to enhance shelf life of foods. Water vapor permeability is an important

property for the edible films to prevent the food spoilage. Water vapor permeability and

antibacterial properties of biopolymers film can be tailored by nanocellulose reinforcement in the

polymer matrix (Dehnad et al. 2014a, Dehnad et al. 2014b). Nanocellulose reinforcement in the

polymer improve the mechanical properties, whereas, reduces the elongation and water barrier

properties required for water barrier films. The nanocomposite biopolymers films are

environmental friendly as compared to their synthetic polymer counterpart (Azeredo et al. 2010).

Highly ordered structure of cellulose nanocrystal improves the mechanical property of film, and

the presence of crystalline nanocellulose believe to increase tortuosity in the film, further,

enormous hydroxyl groups on the cellulose nanocrystal bind the water molecules strongly by

hydrogen bonding as a combined result of slower diffusion process, hence, reduces the water

vapor permeability of the film required for food packaging (Costa et al. 2014, Khan et al. 2010).

24
Nanocellulose can be efficiently reinforced into the polymer matrix by in-situ polymerization for

the preparation of nanocomposite. Mabrouk et al. reported cellulose nanocrystal polymer

composite prepared by miniemulsion polymerization of acrylic monomers in the presence of

cellulose nanocrystal and methacryloxypropyl trimethoxysilane (MPMS) which act as a coupling

agent. Silanol groups on the surface of polymer particles enhance the adsorption of nanocellulose

by hydrogen bonding. During the film formation process (when water evaporates), the physical

interaction may converted into chemical linkage by condensation reaction between surface

silanol groups of the MPMS and hydroxyl groups of nanocellulose, hence, effectively reinforced

the nanocellulose into the polymer matrix (Ben Mabrouk et al. 2014). Ultimate property of the

nanocomposite would depend on proper dispersion, distribution nanocellulosic filler together

with the, interfacial adhesion and the interactions between matrix and nanofillers (Chirayil et al.

2014). Mechanical property of nanocellulose polymer composite increased with the increase of

nanocellulose concentration up to threshold limit then decrease thereafter (Cho and Park 2011).

Interesting properties of polyurethane foams make them ideal for the potential application in

various fields. However, improved properties are required for the specific applications.

Polyurethane foam morphology in terms of cellular morphology, open cell content, foam density,

and mechanical properties such as compressive and tensile properties, and impact properties can

be tailored by nanocellulose reinforcement in the domain structure (Faruk et al. 2014).

5.4 Other applications

Barrier properties of paperboard and paper can be improved by using nanocellulose reinforced

alkyd resin. Smoothness and density of the rough and open structure of uncoated paper surface

25
can be improved by the use of very low loading of nanocellulose in the resin solution. Further,

water barrier properties of the coated paper could be improved due to the sealing of surface and

consequently, creation of surface layer with low porosity. Moreover, water molecules could be

strongly attached with the nanocellulose by hydrogen bonding with the abundant hydroxyl

functionalities on the nanocellulose surfaces, hence, reduces the water transmission through the

nanocellulose containing film (Aulin and Strom 2013).

pH is an important parameter to be measured and monitor for the aqueous solution in the area of

clinical diagnostics, water quality assessment, food processing and bioprocess fields. Cost

effective biocompatible pH sensors can be prepared by aqueous phase synthesis of nanocellulose

and dye conjugate (Chauhan et al. 2014). Farjana et al. reported flexible conductive sensor based

on nanocomposite which was prepared by using bacterial nanocellulose and carbon nanotube

(Farjana et al. 2013).

Polymer dispersion containing crystalline nanocellulose has the potential for the security

printing, and the optical authentication. The printed on a dark paper by using crystalline

nanocellulose containing polymer dispersion shows darker than background with polarizers,

however, brighter if viewed under crossed polarizers (Chindawong and Johannsmann 2014).

Freeze drying method of nanocellulose and sodium montmorillonite produces foam like and

honeycomb like aerogel structure which possesses excellent thermal, mechanical (can retain at

high temperature) and energy absorption capability, and the aerogel could find applications in the

packaging of goods (Donius et al. 2014).

Low cost hybrid films prepared by extrusion of nanocellulose and ZnO suspension with excellent

UV blocking property, lightweight and flexible substrate, could find applications in the UV

26
blocking filed which required transparent substrate (Jiang et al. 2015b). Hybrids aqueous media

of nanofibrillated cellulose and titania nanoparticles can be used for the transparent coatings

where high wear resistance and UV blocking activities are required (Schutz et al. 2012).

Composite paper prepared by using nanocellulose and reduced graphene possesses high

electrical conductivity, excellent mechanical properties in wet and dry condition, and could have

potential application in humid environment as conductors, antistatic coatings, and electronic

packaging (Luong Nguyen and Seppala 2015).

Flexible film prepared by using Zeolite and nanocellulose has excellent capacity to remove the

thiol, hence, the film with excellent mechanical property could be applicable for the packaging of

fruits, foods, and vegetables which releases significant concentrations of odors (Keshavarzi et al.

2015). Nanocellulose and graphene foams having light weight, good combustion efficiency can

be used to improve the energy efficiency of the building (Wicklein et al. 2015). Nanocellulose

can be used to modify the synthetic textile substrate to improve the dye ability of fiber due to the

abundance of hydroxyl groups on the nanocellulose surface and modified fiber could have better

binding to the dye molecules (Nourbakhsh 2015). Conductive carbon fiber can be prepared by

pyrolysis of polyacrylonitrile (PAN) in an inert environment. The electrical conductivity of the

carbon fibers can be enhanced with increasing nanocellulose concentration in PAN matrix

because of the more ordered graphite structure which enhances the movement of the π electrons

(Park, Lee and Kim 2013). Nanocellulose can be used to prepare novel sorbent for the solid

phase micro extraction of biomolecules (Ruiz-Palomero, Soriano and Valcarcel 2014, Ruiz-

Palomero, Soriano and Valcarcel 2015). β-cyclodextrin modified nanocellulose (CD-NC) sorbent

material prepared by using amidation reaction of amine modified nanocellulose is highly

27
efficient and selective against danofloxacin (DAN) which is an antibiotic used to treat animal

diseases (Ruiz-Palomero et al. 2015).

6. Conclusions

In this paper, author reviewed the researches on the nanocellulosic (NC) materials.

Nanocellulosic materials have many interesting properties (such as nontoxicity, biodegradability,

renewability, biocompatibility etc.) which make them ideal candidates for many potential

applications. NC can be extracted from the lignocellulosic biomass by using various methods

which influences their properties. There are enormous potential for the nanocellulosic materials

which includes nanocomposites membrane, hybrid film, hydrogel, aerogel etc. are few of many

to states. Cellulose nanomaterials could have wide applications in food packaging, energy, water

treatment, biomedical filed etc. Further, nanocellulose derived from the bacterial synthesis has

proven as a promising biomaterial for various biomedical applications such as tissue engineering,

drug delivery, wound dressing, cardiovascular applications etc. Author do hope that

comprehensive literature review on nanocelluloses presented in this paper will promote further

researches for the utilization of huge renewable lingocellulosic biomass for the preparation of

nanomaterials which could be useful in diverse applications.

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Figure captions

Figure 1: Number of publication with respect to the publication year based on nanocellulose (source:

web of science; search key word (title): nanocellulose)

Figure 2: Scanning electron microscopy (SEM) images of (a and b) raw CTMP; (c and d) fibers after

acidified sodium chlorite treatment (Ho-CFs); (e and f) fibers after alkali-treated (Al-CFs); and (g and h)

NCFs (Li et al. 2014) [Reproduced with permission, Copyright © 2014 Elsevier Ltd. All rights reserved].

Figure 3: Transmission electron microscopy images showing the morphology of nanocellulose obtained

from various sources a banana rachis b sisal c kapok d pineapple leaf and e coir (Deepa et al. 2015)

[Reproduced with permission, Copyright © 2015, Springer Science+Business Media Dordrecht].

Figure 4: Various common chemical modifications approaches of nanocellulose [PEG: poly(ethylene

glycol); PEO: poly(ethylene oxide); PLA: poly(lactic acid); PAA: poly(acrylic acid); PNiPAAm: poly(N-

isopropylacrylamide); and PDMAEMA: poly(N,N-dimethylaminoethyl methacrylate)] (Lin et al. 2012b)

[Reproduced with permission, Copyright © 2012, Royal Society of Chemistry].

Figure 5: (A) 3D printed small grids (7.2 × 7.2 mm2) with Ink8020 after cross-linking. (B) The shape of the

grid deforms while squeezing, and (C) it is restored after squeezing. (D) 3D printed human ear and (E and

F) sheep meniscus with Ink8020. Side view (E) and top view (F) of meniscus (Markstedt et al 2015)

[Reproduced with permission, Copyright © 2015, American Chemical Society].

Figure 6: a) Digital photographs of a PPy, Nanocellulose, and Graphene oxide (PNG) paper electrode

showing its flexibility during bending. (b) Stress–strain curve for a PNG paper electrode. (c) Cyclic

voltammograms for PNG paper electrodes recorded with two different bending angles, i.e. 0° and 180°,

56
at a scan rate of 20 mV s−1 (Wang et al 2015d) [Reproduced with permission, Copyright © 2015, Royal

Society of Chemistry].

Figure 7: Absorption capacities (Cm) of the silylated sponge (18.9 wt % Si), determined for a collection of

organic solvents (filled symbols) and oils (empty symbols). The sample was deposited at the surface of

the liquid for 5 s (Zhang et al. 2014) [Reproduced with permission, Copyright © 2014, American

Chemical Society]

Figure 8: SEM images of polystyrene latex beads and SIV particles following filtration on Cladophora

cellulose membrane: a) 500 nm beads; b) 100 nm beads; c) 30 nm beads; and d) SIV particles (Metreveli

et al. 2014) [Reproduced with permission, © 2014 Metreveli et al.. Published by WILEY-VCH Verlag

GmbH & Co. KGaA, Weinheim].

Fig 1

57
Fig 2

58
Fig 3

Fig 4

59
Fig 5

60
Fig 6

61
Fig 7

62
Fig 8

63
Table 1: Influence for the source of cellulosic biomass and preparation methods on the lateral

dimension of nano-cellulose

Source of cellulose Lateral dimension Preparation method References

Mengkuang leaves 5-25 nm Acid hydrolysis (El Sheltami, Abdullah and Ahmad 2012)

(Pandanus tectorius)

Banana rachis 10-60 nm Acid hydrolysis (Deepa et al. 2015)

Sisal 20-80 nm Acid hydrolysis (Deepa et al. 2015)

Kapok 20-70 nm Acid hydrolysis (Deepa et al. 2015)

Pineapple leaf 50-150 nm Acid hydrolysis (Deepa et al. 2015)

Coir 40-90 nm Acid hydrolysis (Deepa et al. 2015)

Soft wood pulp 10-20 nm High shear defibrillator (Faruk et al. 2014)

Cladophora sp. green algae 30-40 nm Oxidation (Carlsson et al. 2014)

Cotton linters 39 + 7 nm Acid hydrolysis (Chauhan et al. 2014)

Pineapple leaf fibre 5-60 nm Steam explosion acid hydrolysis (Cherian et al. 2010)

Microcrystalline cellulose 6.96 nm Acid hydrolysis (Cho and Park 2011)

Cellulose powder 20-50 nm High-pressure homogenizer (Chun et al. 2012)

Leaves licuri 5.7-61.6 nm Acid hydrolysis (Costa et al. 2014)

Kraft bagasse pulp 7.5-16.5 nm Acid hydrolysis (El-Wakil et al. 2015)

Gluconacetobacter xylinus 128 nm Bacterial synthesis (Hessler and Klemm 2009)

spruce and pine 5-10 nm Acid hydrolysis (Ishikawa et al. 2015)

Rice straw 1.5-12.6 nm High speed blender (Jiang and Hsieh 2013)

Rice straw 1.4-8.5 nm Acid hydrolysis (Jiang and Hsieh 2013)

64
Rice straw 1.73 ± 0.56 TEMPOa oxidation (Jiang and Hsieh 2013)

Bamboo fiber 10-30 nm Alkali and acid hydrolysis (Jiang et al. 2015)

Rice straw 40-80 nm Acid hydrolysis (Kardam et al. 2014)

Cotton lint <50 nm Acid and mechanical (Nahr et al. 2015)

Maize straw 15-25 nm Acid hydrolysis (Rehman et al. 2014)

Pomelo Fruit Fibers 10-20 nm Acid hydrolysis (Yongvanich 2015)

Citrus waste 10 nm Enzymatic hydrolysis (Marino et al. 2015)

a
TEMPO-2,2,6,6- tetramethylpiperidine-1-oxyl radical

65