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Science of the Total Environment 650 (2019) 1309–1326

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Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Review

An insight into nanocellulose as soft condensed matter: Challenge and


future prospective toward environmental sustainability
KhangWei Tan a, SungKu Heo a, MeiLing Foo b, Irene MeiLeng Chew b, ChangKyoo Yoo a,⁎
a
Department of Environmental Science and Engineering, Center for Environmental Studies, Kyung Hee University, Yongin-Si 446-701, Republic of Korea
b
School of Engineering, Monash University Malaysia, 47500 Subang Jaya, Selangor, Malaysia

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Overview the production of nanocellulose


via sophisticated processing technique.
• Nanocellulose assembly into more
sustainable soft material with unique
properties.
• Emerging applications of 3D nanostruc-
tured nanocellulose soft material in food,
water and energy.

a r t i c l e i n f o a b s t r a c t

Article history: Nanocellulose, a structural polysaccharide that has caught tremendous interests nowadays due to its renewabil-
Received 3 July 2018 ity, inherent biocompatibility and biodegradability, abundance in resource, and environmental friendly nature.
Received in revised form 28 August 2018 They are promising green nanomaterials derived from cellulosic biomass that can be disintegrated into cellulose
Accepted 28 August 2018
nanofibrils (CNF) or cellulose nanocrystals (CNC), relying on their sensitivity to hydrolysis at the axial spacing of
Available online 29 August 2018
disordered domains. Owing to their unique mesoscopic characteristics at nanoscale, nanocellulose has been
Editor: Frederic Coulon widely researched and incorporated as a reinforcement material in composite materials. The world has been con-
suming the natural resources at a much higher speed than the environment could regenerate. Today, as an upris-
Keywords: ing candidate in soft condensed matter physics, a growing interest was received owing to its unique self-
Nanocellulose assembly behaviour and quantum size effect in the formation of three-dimensional nanostructured material,
Soft condensed matter could be utilised to address an increasing concern over global warming and environmental conservation. In
Food spite of an emerging pool of knowledge on the nanocellulose downstream application, that was lacking of
Water cross-disciplinary study of its role as a soft condensed matter for food, water and energy applications toward en-
Energy
vironmental sustainability. Here we aim to provide an insight for the latest development of cellulose nanotech-
nology arises from its fascinating physical and chemical characteristic for the interest of different technology
holders.
© 2018 Elsevier B.V. All rights reserved.

⁎ Corresponding author.
E-mail addresses: energizer@khu.ac.kr (S. Heo), mei.foo@monash.edu (M. Foo), irene.chew@monash.edu (I.M. Chew), ckyoo@khu.ac.kr (C. Yoo).

https://doi.org/10.1016/j.scitotenv.2018.08.402
0048-9697/© 2018 Elsevier B.V. All rights reserved.
1310 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1310
2. From native cellulose to designed functionalities . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1311
3. Toward environment sustainability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1315
3.1. Food . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1315
3.2. Water . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1317
3.3. Energy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1320
4. Summary and outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1323
. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1323
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1323

1. Introduction Although study on nanocellulose can be traced back to 1960s (Rånby,


1951), where nanocellulose was isolated via a top-down approach
While economy is rapidly expanding in most emerging countries, is- from bulky cellulosic material using concentrated hydrochloric acids
sues coupled with higher population and improved living standard had and sulfuric acids, the study has been stagnant and only accelerated
created foreseeable tension on demand among food, water and energy. after 1999. Before this, only few academic reports were received
It is crucial for more sustainable valorisation of resources, for instance, throughout the years (Fig. 1a). Concerning its excellent mechanical
nanocellulose, to address the core challenge in environmental sustain- properties, much work had been focused on composite materials pro-
ability. Recently, focus has been shifted toward its unique physical and cessing and properties, after a tremendous study addressing its extrac-
chemical properties as a soft condensed matter, concerning its behav- tion since the early '00s (Fig. 1c & d). It was also observed a notable
iour at nanoscale in the forms such as liquid crystals, membranes, gel shift toward medicine, energy and environmental preservation in the
and emulsions (Nystrom et al., 2018; Fatona et al., 2018; Urbanski past 10 years. Driven by strong global nanocellulose market demand,
et al., 2017; Lubensky, 1997). They share fascinating characteristic which stood at USD 54.19 million in 2014 and USD 87.5 million in
such as unique self-assembly behaviour in liquid medium governed by 2016, was expected to reach approximately USD 699.6 million in 2023
molecular forces and quantum mechanics, can be extensively studied by a phenomenal compound annual growth rate (CAGR) of 33.8%
via wet experiment, molecular dynamic simulation or theoretical calcu- (Transparency Market Research, 2015; Global Market Insights, 2018).
lation for a wide range of unique applications (Kolle and Lee, 2017; This is well reflected in Fig. 1b which shows a substantial growth of in-
Brandt et al., 2014). ternational grants derived mainly from US Patent & Trademark Office,
Nanocelluloses are promising structural polysaccharides at nano- the European Patent Office, the Japan Patent Office, the World Intellec-
scale that can be strategically extracted from any cellulosic organic mat- tual Property Organization and the UK Intellectual Property Office. A
ters principally through chemical hydrolysis, mechanical disruption, positive dynamic link is recorded since 2000, whereby only two lags
enzymatic, or combination of two (or more) approaches (Lindström, were observed from 2004 to 2005 and 2007 to 2008, due to oil prices
2017; Djalal Trache et al., 2017; C. Endes et al., 2016). Depending on crash and financial crisis, respectively (Fig. 1b). CNF segmented the
the process, they would therefore appear in a variety of characteristic highest portion followed by NCC in the global market, while the remain-
shape with diverse surface chemistry and crystallinity, that largely de- ing goes to bacteria cellulose (BC) that contributed a few percentages
termine their role in later applications. In general, nanocellulose could points to the total. Geographically, North America and Europe were
be categorised into two groups, one with longer semi-crystalline fibril- the main contributors which make up of approximately 60% of market
lar structure called cellulose nanofibers (CNF, or nanofibrillated cellu- share in 2014, a result of strong demand over biodegradable antimicro-
lose), while the other one with highly crystalline structure in the bial packaging materials in food and beverages industry, high quality
name of cellulose nanocrystal (CNC, or nanocrystalline cellulose). CNFs paper products and personal health care. Looking at most cellulosic bio-
are rich in plant cell wall, making the main components in plant micro- mass is originated from Asia Pacific region, it was expected that it would
fibrils that provide strength and stiffness to plant anatomy. They are largely increase its market share in the coming decade. On top of that,
long cellulose polymer with few microns in length, constituted of both the more stringent regulations by administrative bodies concerning in-
amorphous and crystalline region. Amorphous regions (or disordered dustrial procedure toward greenhouse gas emission and non-
regions) are highly susceptible to hydrolysis that can be steadily re- biodegradable materials has further accelerated the research activities
moved to obtain crystalline region of NCC upon phase segregation. in the Asia Pacific region. It is foreseeable more promotional activities
NCC are rod-shape (or needle-shaped) highly crystalline particles hav- and a clearer product positioning will be the strategic core in the coming
ing at least one dimension in lesser than 100 nm (Ruiz et al., 2000; decade for the market prominent players of nanocellulose materials, in-
Brinchi et al., 2013). They are probably the smallest biological active cluding CelluForce Inc., Fpinnovations, American Process Inc., Nippon
building block of cellulose, suggesting supreme mechanical characteris- Paper Group Inc., CelluComp, Asahi Kasei, Daicel, Asahi Kasei Corpora-
tic due to their highly crystalline structure, on top of their inherent bio- tion, and BASF AG; also, not neglecting the contribution from the labora-
compatibility and biodegradability (Habibi et al., 2010). tory scale manufacturers, including Innventia, Borregaard and Stora
Research activities concerning cellulose nanotechnology had Enso.
attracted tremendous attention over the past decade which is well Extended from its more straightforward use as an enhancing com-
reflected on the rapid increase of scientific publication and patents ponent for composites, study had recently moved forward to re-define
granted internationally (Fig. 1a & b). Initially, literature search was con- its role as a soft condensed matter in a multiphase system. Albeit of its
ducted via Elsevier Scopus using a more general term “nanocellulose” extra-ordinary performance, it has still remained a challenging task to
resulted in a limited outcome due to inconsistent nomenclature used understand its fundamental principle in liquid system. Also, it's fascinat-
across the discipline. For comparison, literature search was again con- ing behaviour induced sol-gel transition and chiral inversion has seldom
ducted using multiple search terms i.e. “nanocellulose”, “nanocrystal- been discussed. These was of upmost importance in the current horizon
line cellulose”, “cellulose nanocrystal”, “cellulose nanofiber”, “cellulose of nanocellulose product development. For instance, its liquid crystal
nanofibril”, “cellulose whisker” and “cellulose nanowhiskers”, where a self-assembly behaviour in the formation of chiral nematic film created
significant increase of publication number was observed (Fig. 1a). possibility for security papers (Derek G. Gray, 2016; Jan PF Lagerwall
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1311

Fig. 1. The development of nanocellulose in the past two decades, (a) Annual scientific publication since 2004; (b) Annual international patents granted since 2000; (c) The development of
NCC distributed against subject areas; (d) Total number of Publication against countries and subject areas.
Data analysis was extracted form Scopus on 10 May 2018.

et al., 2014); Paraffin encapsulated by CNF via Pickering emulsion often obtained through a top-down hydrolysis approach in which ligno-
method for the making of phase change materials to conserve solar en- cellulose, lignin and hemicellulose were removed on a layer-to-layer
ergy (Li et al., 2017a, 2017b); fabrication of magnetic-cellulose base basis (Fig. 2). Conceptually, it consisted of four steps, i.e. (i) pre-
polymeric ionic liquid for effective anionic dye biosorption (Beyki treatment of cellulosic fibres via physical/mechanical methods involv-
et al., 2016); CNF aerogel-based water/oil/water microreactor for highly ing grinding, screening, washing and cooking to remove dust, oily con-
efficient molecular or ions extraction and separation (Li et al., 2017a, tent and coarse particles on material surface (ii) isolating the most inner
2017b); and CNC-based nanocarrier for enzyme immobilization (Cao cellulose fibrous content from lignocellulosic body consisted of glyco-
et al., 2016). protein/pectin/hemicellulose in the plant primary wall, and lignin/
In this review, we aim to cover literature pertaining to the most cur- hemicellulose in the macrofibrils (or secondary plant cell wall), by
rent development of nanocellulose as a soft material that make a signif- means of chemical, mechanical or enzymatic treatment, (iii) fragmenta-
icant contribution to food, water and energy applications. Despite its tion of cellulose fibrils in the microfibrils into CNF or CNC through hy-
promising characteristic, nanocellulose is still at its early stage of devel- drolysis or mechanical destruction, and (iv) Strategies to
opment as compared to other elite nanomaterials, for instance, carbon nanocellulose surface modification for tailoring of the interfacial inter-
nanotube and graphene, where 134,174 and 114,212 related scientific actions that fundamentally change its fluid-like behaviour. This final
reports were received to date (May 2018), respectively. Although step is rather sophisticated in the current research horizon for designing
nanocellulose was generally regarded as environmental benign and new soft matter system.
non-toxic to human, more work has to be done to overcome the issue Ideally, nanocellulose can be obtained from any cellulosic fibres.
of public acceptance from the end user (Adewuyi et al., 2018; Menas Some worth mentioning considered the growing environmental con-
et al., 2017; Kovacs et al., 2010). cern over the end-of-life disposal challenges from the agricultural
waste, i.e. oil palm empty fruit bunches (Zianor Azrina et al., 2017;
2. From native cellulose to designed functionalities Foo et al., 2017; Shanmugarajah et al., 2015), bamboo pulps (Wang
et al., 2016), corn fibres (Hernandez et al., 2018; Xu et al., 2018a), flax
Nanocelluloses are carbohydrate polymer at nano-scale constituted stalks (Istomin et al., 2016), jute fibres (Jabbar, 2017) and rice husks
of repeating units of two anhydroglucose linked by a β (1 → 4) glyco- (Islam et al., 2018; Kalita et al., 2015). Nevertheless, it could be more
sidic bond (Eyley and Thielemans, 2014). Through a complex intramo- conventionally extracted from wood pulps (Liimatainen et al., 2013;
lecular hydrogen-bonding network the cellulose chains assemble and Sheikhi et al., 2016), cotton fibres (Theivasanthi et al., 2018), recycled
form into a highly stable acid-resistant crystalline structure (Fig. 2). It papers (Mohamed et al., 2015) and Whatman filter paper (Sadeghifar
retained much of the native cellulosic structure originated from the et al., 2011).
sources, and the particles surface characteristics were determined by Nanocellulose are hydrophilic insoluble nanoparticles in water. They
its isolation strategies (Djalal Trache et al., 2017). These would therefore are poorly dispersed in nonpolar solvent, as well as nonpolar polymer
influence its nanomechanics properties as a soft material, and subse- matrix for nanocomposite preparation. Owing to the intramolecular hy-
quently contribute to its final application. Nanocellulose was most drogen bonding contributed by the three hydroxyl groups on native
1312 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

Fig. 2. Illustration of nanocellulose production from raw cellulosic fibrous materials, extraction methods to molecular structure modification for better functionality.

anhydroglucose units, nanocellulose are likely to aggregate in both and tissue drape (Geyer et al., 1994; Solway et al., 2010). For example,
polar and non-polar medium and subsequently resulted in a sol-gel or- polyvinyl alcohol was mixed with bacterial cellulose extracted from
ganization. This could be managed by the introduction of high energy bacterium Acetobacter xylinum to form a soft biocompatible material
mechanical irritation, such as high-pressure homogenizer or ultrasonic showing encouraging mechanical properties similar to that of a cardio-
cavitation (Beck et al., 2012; Khoshkava and Kamal, 2013). However, vascular tissue (Millon and Wan, 2006). The promising tensile proper-
it was most often tailored by certain chemistries to alter their function- ties and relaxation rate allow a faster recovery during cardiac cycle,
alities, through molecular grafting or substitution of hydroxyl groups on contributed by the high elastic modulus from bacterial cellulose and ex-
cellulose surface (Fig. 2). As such, it was traditionally having a unique tensive hydrogen bond formation with polyvinvyl alcohol, suggesting
contribution as a biomaterial in some medical areas e.g. wound healing them a suitable material for aorta tissue replacement. Bacterial cellulose
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1313

can also be mixed with polyethylene glycol to obtain foam structure via behaviour in water (Honorato et al., 2015). Above a critical concentra-
a simple freeze-drying process (Cai and Kim, 2010). The well intercon- tion, the viscosity was increasing with increase of concentration, sug-
nected porous network structure was evidenced under scanning elec- gesting a new category of reliable soft materials in high functioning
tron microscope and for the first time its biocompatibility was sol-gel (Mendoza et al., 2018a, 2018b; Pääkkönen et al., 2016), aerogel
confirmed. Qualitatively, as observed from scanning electron micro- (Afsahi et al., 2018) and Pickering emulsion (Gestranius et al., 2017)
scope, the cells adhered, well spread and proliferating over the compos- fabrication. The TEMPO-mediated nanocellulose can be used to produce
ite surface, suggesting it a promising material for wound dressing and monodispersed silver nanoparticles through strong ion interaction be-
tissue regeneration scaffold application. Later on, Alam and his group tween cellulose carboxylate groups and silver ion precursor (Ifuku
studied bacterial cellulose-koalin composite to realise its structure- et al., 2009). However, TEMPO-oxidized nanocellulose was more fre-
property relationship for wound healing (Wanna et al., 2013; Véliz quently discussed for medical applications (Luo et al., 2013) owing to
et al., 2014). Supported by both experimental and modelling research, its high purity and selectivity. In addition, Alam and his group demon-
the authors suggested the non-linear strength of blood attachment strated that a TEMPO-oxidized bacterial cellulose could be further mod-
was related to several factors including material surface topography ified with amino acid such as alanine, glycine and proline, which
that was highly determined by the faction of bacterial cellulose in the showed a higher strength and toughness as compared to pure bacterial
composite material. For bone regeneration, bacterial cellulose has cellulose. Molecular dynamic simulation suggested that more hydrogen
realised its role to provide microscopic pore structure to facilitate oste- bond was formed among bacterial cellulose, attaining more intermolec-
oblast ingrowth and the formation of mineralised tissue (Zaborowska ular energy resulted in better mechanical strength which is beneficial in
et al., 2010). It was observed that MC3T3-E1 osteoprogenitor cells the current development of biomaterial (Pahlevan and Alam, 2016;
were well clustered within the pores in a scaffold, and formed a denser Pahlevan et al., 2018). The successful fabrication of amino acid modified
mineral deposit than the control. For in vitro degradation and cytotoxic- TEMPO-oxidized cellulose can be further enhanced with silver nanopar-
ity of bacterial cellulose in bone regeneration can be referred to Xi et al. ticles to acquire antibacterial activity (Huang et al., 2013). The study
(2009). showed an excellent antibacterial activity against Staphylococcus aureus
Cellulose derivative could be altered via covalent modification, such and Escherichia coli, through observation over bacteria growth on a LB
as esterification and etherification for a wide range of industry applica- agar plate. A recent study suggested that rapid cooling might enhanced
tion (Fig. 2). For example, microsuspension polymerization of poly hydrogen bond energy and thermal stability of suspended TEMPO-
(methyl methacrylate) using methycellulose and CNC (Kedzior et al., oxidized NCC (Mhd Haniffa et al., 2017). In contrast to other major ap-
2017); a highly stable aqueous foam stabilised by methycellulose and proaches such as mechanical and enzymatic method which showed a
CNC (Zhen Hu et al., 2016); hydroxyethyl cellulose hydrogels for trans- relatively lesser impact are not discussed in this section.
dermal isoliquiritigenin delivery (Kong et al., 2016). They could possess Nanocellulose with reduced degree of polymerization are principally
thermoplastic characteristics by carefully adjust the degree of substitu- more inert in water. They form an unordered isotropic suspension at a
tion or by molecular substitution (Yano et al., 2018; Agustin et al., 2016), sufficiently low concentration, and phase change into an ordered ar-
or pH-responsive with a “greener” footprint (Li et al., 2015a, 2015b). rangement when a critical concentration was met. Despite recent prog-
Other important addition including fluorescence modification for poly- ress in cellulose nanotechnology, the mechanism behind the chirality
mer tracking (Bombeck et al., 2017; Navarro et al., 2016), environmen- inversion of filamentous cellulose colloids remained mysterious, as
tal friendly hydrophobization procedure for potential food application well as the interchange between gelation and liquid crystal was still
(Hu et al., 2017; Shang et al., 2018), silylation for industrial effluent re- contentious (Nystrom et al., 2018; Gray, 2018). The observed chirality
mediation (Ufodike et al., 2018; Laitinen et al., 2017; Pacaphol and Aht- was often a result of particles morphology and surface chemistry
Ong, 2017), cationization for composite material fabrication (Tang et al., (Fig. 4). Owing to the large number of possible functional groups on
2018a, 2018b; Tian et al., 2017; Yang and van de Ven, 2016), and finally nanocellulose surface, nanocellulose was mobilising in electrostatic sta-
polymer grafting toward designed properties such as anti-bacterial pho- bilization following Brownian motion, showing in a fingerprint pattern
todynamic inactivation efficacy (Dong et al., 2018), thermo-responsive of chiral nematic order. This order could be preserved upon evaporation,
(Khine et al., 2018), enhanced thermal stability (Lavoine et al., 2017), suggested a promising optical and photonic material for various appli-
biomimetic reversible heat-stiffening property (Cudjoe et al., 2017) cation. Theoretically, it was rather a complicated process which went
and improved barrier properties (Espino-Pérez et al., 2018). through biphasic and chiral nematic phase, forming a thixothropic gel
Fig. 3 illustrates three most commonly used nanocellulose extraction with very low water content before completely dried into a solid chiral
process which contributes to alter nanocellulose chemical structure and nematic film (Nystrom et al., 2018; Gray and Mu, 2015). Other than the
particle fragmentation. Sulfonation occurred during sulfuric acid hydro- own characteristic of the nanocellulose itself, it was suggested that the
lysis via esterification by dissociating hydroxyl groups at C2, C3 and C6 concentration, the rate of evaporation and the ionic strength are the
on the glucosyl ring (Al-Dulaimi and Wanrosli, 2017). They are partially main factors governing the chiral nematic pitch as observed by polar-
water-soluble depending on degree of substitution that could be feasi- ized light microscopy (Gray, 2018). However, the thermodynamic
bly controlled over acid concentration, duration, etc. during hydrolysis governing the chiral interaction during film formation remain unknown
procedure. Owing to the anionic sulfate half ester groups, they form sta- to date. It was also suggested that the relaxation of shear-induced orien-
ble colloidal suspension with desirable optical properties suggesting tation may contribute to liquid crystal structure via an intermediate
them an interesting candidate for transparent composite material twist-bend state. This was highly relied on the uniformity of the ex-
upon drying (Reid et al., 2017; Liimatainen et al., 2013). It is worth men- tracted nanocellulose, could be another challenging aspect in the cur-
tioning that the excellent mechanical properties of the CNF extracted via rent research scenario.
sulfonation of 2,3-dialdehyde cellulose was independent of its sulfate Nanocellulose are non-surface active, yet could be tailored via nu-
content, and the periodate used in the treatment could be practically merous hydroxyl groups on the cellulose surface to modulate their in-
recycled, suggesting a more cost-effective and greener approach for herent hydrophilicity. This unique thermo-mechanical characteristic
nanofibrillation (Liimatainen et al., 2013). TEMPO-mediated (or showed great promise to stabilize interface by forming emulsion and
2,2,6,6-Tetramethylpiperidine-1-oxyl-mediated) oxidation is another foam at nano-scale that anchored consumers' need heavily in daily
major approach for nanocellulose extraction especially for CNF (Isogai life. Several factors have been identified to construct a stabilised nano-
et al., 2011; Barud et al., 2008). Unlike other approaches, TEMPO- scale multiphase system, but principally relying on two i.e. the surface
mediated oxidation is highly selective and only react with hydroxy- chemistry and shape of nanocellulose (Fig. 5). For liquid-liquid system,
methyl group at C6 on the glucosyl ring (Habibi, 2014; de Nooy et al., it was advised that the nanocellulose should be 10 times smaller than
1994). They are generally thixotropic and showing a shear-thinning the droplet to form a successful Pickering emulsion, and they are
1314 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

Fig. 3. The illustration of major approaches in nanocellulose production. (a) Chemical Approach via acid hydrolysis (Adapted with permission from Foo et al. (2017)); (b) Mechanical
Approach via high intensity ultrasonic cavitation (Adapted with permission from Li et al. (2016)); (c) Enzymatic Approach via cellulase hydrolysis (Adapted with permission from Cui
et al. (2016)).

extremely stable in most cases with very low nanocellulose concentra- the adsorption energy to the interface can be quantitatively described
tion (Yang et al., 2017; Thompson et al., 2017). Fig. 5a showed a rela- in Eq. (1):
tionship between contact angle of a spherical particle to the formation
of oil-in-water (or water-in-oil) emulsion, while Fig. 5b showed more ΔG ¼ −πR2 γð1−j cosθjÞ2 ð1Þ
contact area could be obtained by a bending CNF/CNC for better stabili-
zation of Pickering emulsion. Fig. 5c illustrated the distribution of spher- where R is the radius of the particles, γ is the interfacial tension and θ is
ical particles on the droplet curvature in comparison to CNC/CNF the contract angle. For rod-like CNC or a much longer CNF, Eq. (1) can be
stabilised Pickering emulsion (Fig. 5d). Fig. 5e, f and g showed SEM revised into Eq. (2):
image of actual Bacterial cellulose nanofibers, CNC and spherical silica
stabilised Pickering emulsion, respectively. Noting that the energy re- ΔG ¼ −lbγ ð1−j cosθjÞ2 ð2Þ
quired to desorb from the interface is much larger than a conventional
surfactant (Capron et al., 2017), forming a solid physical barrier that where l is the length of nanocellulose and b is the width. In comparison
are more reliable than a thermodynamically stable macroemulsion or to most colloidal system which usually a spherical particle was
kinetically stable nanoemulsion (Tan et al., 2016). The expression of employed, a Pickering emulsion system stabilised by nanocellulose is
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1315

Fig. 4. (a) Possible fragmentation of cellulose nanofibril into shorter CNC; (b) cellulose nanofibril before and (c) after acid hydrolysis; (d) Segment length distribution; Illustration of CNC
assembly behaviour in liquid medium (e) initial cellulose nanofibril (f) breakdown (g) scattering (h) assembly (i) nematic phase (j) smectic phase and (k–l) cholesteric or chiral nematic
phase.
(Reproduced with permission from Nystrom et al. (2018)).

much effective as larger contact area was provided in the same volume, rate at increased temperature require much innovation on food storage
owing to much diversity of particle shape and morphology could be ob- should come in a more affordable price and in a more environmental
tained via different extraction technique from various raw materials friendly manner (Hammond et al., 2015). It also requires more attention
(Fig. 6). to increase food shelf-life of safety, as well as the ability to maintain food
nutrition capacity (Vilarinho et al., 2018).
3. Toward environment sustainability Fine particle technologies have been well applied in food industries
(Faridi Esfanjani and Jafari, 2016; Sahoo et al., 2016; Dahmash and
There are huge motivations and incentives at the present time. Mohammed, 2015; Ogi et al., 2014; Inoue, 2011), attributed mainly on
Water is the core for sustainable socio-economic development. Observ- their extraordinary surface activities and mechanical properties. Re-
ing the fast population growth from the emerging economies, that is an cently, focus had been shifted from Petrochemical base derivatives to
urgent need to balance its commercial demands for better community nanocellulose, a natural-based material that could possibly change the
usage. Also, a greater demand on food over the fast population growth current industrial approach which often claimed to be not environmen-
in the region, not to mention the extreme weather, a result of climate tal friendly and potentially poisonous. For example, food packaging,
change that had further constricted the scenario. In this section we which required innovation on its manufacture on top of its traditional
reviewed the latest development of more sustainable nanocellulose function to prevent deterioration of food, drink, health care or supple-
soft materials for emerging application in food, water and energy. ment during transportation and storage (Garavand et al., 2017;
Bharimalla et al., 2017; Li et al., 2015a, 2015b; Abdul Khalil et al.,
3.1. Food 2016). The current technology relied on fossil-derived synthetic plastic
materials prepared from hydrocarbon polymerization process are not
Food insecurity as a result of rapid population growth is worsening eco-friendly and sustainable. It drained too much of social cost, and
when the crop yield dropped dramatically due to climate change often ended in massive environmental issue (Garavand et al., 2017;
(Campbell et al., 2016; Benegiamo and Cirillo, 2018). It was also noticed Johansson et al., 2012). This could be overcome by employing
that eventhough more effort was paid to increase crop yield, yet produc- biopolymer-based materials, however, it had seldom provided a satis-
tion on livestock, fisheries and pests were much lagging behind that re- factory barrier property against oxygen, water, vapor, oil, grease and mi-
quiring a strategy-based application ion innovative livestock production croorganism as compared to glass, aluminium and tin. Nanocellulose
and delivery (Dehghani et al., 2018; Ramachandraiah et al., 2018). It had recently arisen in the form of coating, or self-standing thin film to
was realised that food price, trade flow and food access would likely provide outstanding barrier properties owing to its well-controlled
to impact a stable society in the next two decades (Nelson et al., polymer matrix pore size in governing gas permeability, as well as in liq-
2014a; Nelson et al., 2014b). For example, higher microbial growth uid diffusion. The challenge in coat/film production often relied on the
1316 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

Fig. 5. (a) Interaction of spherical particles on liquid-liquid interface (Adapted with permission from Binks (2002)); (b) Comparison of bending (or not) CNF/CNC positioning to droplet
curvature (Adapted with permission from Capron et al. (2017)); (c) Illustration of spherical and rod-shaped particles positioning and stabilizing an emulsion (Adapted with permission
from Capron et al. (2017)); (e) bacterial cellulose nanofibers Pickering emulsion (Adapted with permission from Kalashnikova et al. (2012)); (f) CNC Pickering emulsion (Adapted with
permission from Kalashnikova et al. (2012)); (g) Silica Pickering emulsion (Adapted with permission from Zanini et al. (2017)).

transformation of polymer hydrocolloids into well-defined liquid- cost of study, and advanced analytical instrument for soft matter charac-
crystalline polymer, in the presence or absence of solvent, a sophisti- terization at micro- or nano-scaled level. Nanocellulose is an excellent
cated process to control nanocellulose self-assembly behaviour to the food stabilizer. They are generally recognized as being safe (GRAS)
formation of anisotropic solid film as a final product. Some recent suc- (Ferrer et al., 2017), could be well dispersed in water and self-
cessful cases including: transparent nanocomposite film with reduced assembly in response to electrostatic attraction among the hydroxyl
air permeability achieved by increased shear viscosity of the as- groups leading to the organization of sol-gel (or aerogel) structure, or
prepared composite suspension with increased NCC loading (Tang formation of steric barrier between oil and water interface which
et al., 2018a, 2018b) (Fig. 7a); Solvent casting of chitosan/CNC/ greatly enhance the colloidal stability against physical coalescence or
carboxymethyl cellulose colloids for excellent barrier against grease, chemical oxidation (De France et al., 2017; Fujisawa et al., 2017). They
water and oil (Chi and Catchmark, 2018); MMT-stacking in could be further tailored via surface modification for different purposes
nanocellulose network for lowest possible water vapor permeability (Zia-ud-Din et al., 2017). In the past decade, much attention had been
by increasing structure tortuosity (Garusinghe et al., 2018) (Fig. 7b); paid toward its contribution in food microstructure for elevated mouth-
free-standing nanocellulose film obtained via simple dying owing to feel or bioactive preservation, nevertheless the latest breakthrough was
their strong inter-fibrillar hydrogen bonding formed in colloidal sus- rather a phenomenon fundamentally at nano dimension. Some notable
pension (Faradilla et al., 2017); dense nanocellulose coating layer to recent advance including: (Fig. 7e) CNF aerogel formation via toughen-
provide improved strength, lower oxygen and water vapor permeability ing mechanism of freezing and thawing process (inspired by the making
(Herrera et al., 2017) (Fig. 7c); and excellent hydrophobic film via one- of traditional Chinese tofu) showed high porosity of 98%, low density of
pot method from sol-gel nanocellulose-silica (Le et al., 2017) (Fig. 7d). 0.018 g/cm and high surface area above 30 m2/g with no special reactors
Cellulose has a long history in food application (Gómez et al., 2016; involved (Li et al., 2017a, 2017b); sunflower oil stabilised by CNF as an
Dudefoi et al., 2018). Back in 1980s, Turbak and his group developed a effective Pickering emulsion stabilizer (Costa et al., 2018); (Fig. 7f) edi-
series of food products using nanocellulose mainly as a food stabilizer ble food packing via casting film-forming CNC emulsion (Pereda et al.,
owing to its excellent wettability to water over oil, or food additive 2014); (Fig. 7g) promising antimicrobial characteristic over four tested
such as whipped topping, salad dressing and sauces (Turbak et al., microorganism (i.e. Escherichia coli, Staphylococcus aureus, Bacillus
1983; Turbak, 1984). However, the development had seemed stagnant subtilis and Saccharomyces cerevisiae) observed from oregano essential
in 1990s, and only attract considerable attention back in 2000s triggered oil Pickering emulsion stabilised by CNC (Zhou et al., 2018); and a stable
by the rapid development of nanotechnology, a result of more mature high internal phase Pickering emulsion (N80%) could be achieved at
nanocellulose extraction technology that significantly bring down the very low CNC concentration (Chen et al., 2018).
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1317

Fig. 6. The surface morphology of NC (a) NCC from pine wood, TEM (Adapted with permission from Ditzel et al. (2017)); (b) NCC from oil palm empty fruit bunches, FESEM (Adapted with
permission from Foo et al., 2016; (c) NCC extracted from spruce wood, SEM (Adapted with permission from Kunaver et al. (2016)); (d) NCC from sugar palm fibres, AFM (Adapted with
permission from Ilyas et al. (2018)); (e) nanocellulose from spent tea residue, TEM (Adapted with permission from Chen et al. (2018)); (f) CNF from Halocynthia roretzi, TEM (Adapted
with permission from Saito et al. (2013)); (g) PEO/CNF nanofiber mat, FESEM (Adapted with permission from Xu et al. (2014)); (h) CNF-Fe3+ nanogel, FESEM (Adapted with permission
from Dong et al. (2013)); (i) SC, TEM (Adapted with permission from Ram and Chauhan (2018)); (j) SCN, AFM (Adapted with permission from Evdokimova et al. (2018)); (k) BC from
Gluconacetobacter xylinum, SEM (Adapted with permission from Qiu et al. (2016)); (l) BC from Gluconacetobacter hansenii strain ATCC 23769, FEG-SEM (Adapted with permission from
Oliveira Barud et al. (2015)).

3.2. Water studied and implemented worldwide. The available technologies hold
different advantages and disadvantages, and served according to budget
Along with demographic dividend, a rising tension among industrial and effectiveness. Among all, activated carbon has been extensively
demands on water resources threaten a sustainable socio-economic de- used in an adsorption process due to its high removal efficiency, ease
velopment in most of the developing countries. Water is one of the most of handling and reliable operating process (Wong et al., 2018; Inyang
important resources in food production, energy and healthy ecosystem et al., 2016; Yu et al., 2016). However, the manufacture and the regener-
(Helmstedt et al., 2018; Reddy et al., 2018; Lee et al., 2017). It is also cru- ation of activated carbon is not cost and energy effective which may
cial to provide basic sanitation to ensure maternity in dignity (Munabi- raise a considerable attention to environment and human society in
Babigumira et al., 2017; Turck, 2011). Coupling with tremendous eco- long term. Cellulose based nanomaterials have recently emerged to be
nomic growth in Asia-Pacific region driven by several fast-growing a good alternative thanks to the rapid development of cellulose nano-
economies, wastewater treatment and desalination face unprecedented technology since past decade (Putro et al., 2017; Voisin et al., 2017). It
challenge dealing with widespread pollution from urban and industrial was first introduced in the form of native cellulose nanoparticles, dem-
activities. This could be also the main cause of climate change (Koop and onstrated excellent adsorption capacity due to its inherent hydrophilic-
van Leeuwen, 2017; Larsen et al., 2016; Lam et al., 2015). Water treat- ity and active surface functionality. Adsorption is a spontaneous
ment due to the presence of a variety of contaminants such as heavy phenomenon where contaminants (adsorbates) adsorbed onto
metal ions, dyes, polymers, pesticides and detergents, had been widely nanocellulose (adsorbents) driven by different forces of attraction
1318 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

Fig. 7. (a) Image of chitosan/guar gum/CNC optical transparent nanocomposite film (Adapted with permission from Tang et al. (2018a, 2018b)); (b) Cross-sectional SEM image of
nanocellulose-montmorillonite composite illustrating imaginary water and oxygen molecules permeating pathway (Adapted with permission from Garusinghe et al. (2018)); (ci-iii)
Plasticized nanocellulose coating via layer-by-layer technique (Adapted with permission from Herrera et al. (2017)); (d) Illustration of hydrophobic nanocellulose-silica film
fabrication process via a facile one-pot method (Adapted with permission from Le et al. (2017)); (e) Fabrication of highly porous cellulose aerogel inspired by the making of traditional
Chinese tofu (Adapted with permission from Li et al., 2017); (f) optical microscope image of chitosan/glycerol/olive oil emulsions containing 1 wt% nanocellulose (Adapted with
permission from Pereda et al. (2014)); (gi-iv) SEM images of E. coli and S. aureus treated with OEO Pickering emulsion for 3 h (Adapted with permission from Zhou et al. (2018)).

mainly in the categories of physisorption and chemisorption adsorption can also be calculated from the model (Ho, 2006). The ad-
(Mohammed et al., 2018; Putro et al., 2017). Principally, physisorption sorption equilibria data can also be studied via isotherm models, partic-
involves weak intermolecular forces such as Van der Waals forces that ularly relying on Langmuir isotherm which suggests a monolayer
contaminant molecules concentrated on adsorbents surface without surface adsorption, or a Freundlich isotherm which indicates a hetero-
significant change of electronic orbital patterns, whereas, chemical geneity of adsorbents. Owing to the assumption that one adsorbate mol-
bonds formed among adsorbates and adsorbents in a chemisorption ecule only react with one sorption site and the adsorption energy is
process that usually suggest a higher enthalpy (80–800 kJ/mol, as com- constant due to the surface homogeneity in a Langmuir isotherm
pared to physisorption which is usually b80 kJ/mol). The detailed mech- model, it was often correlated to a thermodynamic study to further de-
anism was can be studied from the kinetic or isotherm point of view. fine the adsorption nature. For physisorption, the adsorption affinity ob-
Among various kinetic models targeting liquid-solid phase sorption sys- tained from the Langmuir equation decreases with increase of operating
tem, the sorption kinetic data was often received via Lagergren pseudo- temperature, whereas, the adsorption affinity increases with increase of
first-order and pseudo-second-order equations. The general expression operating temperature due to chemisorption endothermic nature. In
of pseudo-first-order equation as proposed by Lagergren in 1989 de- contrast, Freundlich isotherm is an empirical model which is helpful
scribed the rate of occupation against time, based on the assumption to provide phenomenological information to determine a favourable
that one adsorbate molecules would only react with one sorption site adsorption. An inclusive work can be found from a recent report
on the adsorbent (Ho, 2004; Ho and McKay, 1998; Lagergren, 1989). (Putro et al., 2017) which a comprehensive list of sorption study against
The later development of various second-order rate expression sub- Langmuir and Freundlich isotherm was provided.
jected to different assumption make a distinct difference on the “one- Nanocellulose can be further tailored on its semi-crystalline struc-
site-occupancy” rule, yet, it was often referring to a chemisorption pro- ture to seek more desired aspect ratio, physical accessibility, chemical
cess involving covalent forces as a result of electron exchange between accessibility and quantum effect. However, due to its unique and rather
adsorbate and adsorbent (Ho, 1999). It appeared that majority of the complex colloidal behaviour at nanoscale, the recovery of spent
current studies using nanocellulose as adsorbent are following nanocellulose after adsorption can be costly and practically challenging
pseudo-second order (Mohammed et al., 2018; Putro et al., 2017; in large-scale application. One option is to integrate modified
Hokkanen et al., 2016), a result of vigorous adsorbate-adsorbent inter- nanocellulose into composite material that can be easily recovered
action driven by multiple hydroxyl reactive groups or modified groups and regenerated via physical or chemical methods. It can be therefore
on nanocellulose (Eyley and Thielemans, 2014). It was also suggested fixed into a fixed bed filtration column for large volume continuous pro-
that a pseudo-second order kinetic model could be developed without cess (Xu et al., 2018a, 2018b; Karim et al., 2017; Mohammed et al.,
knowing the equilibrium capacity from the experiment, and the initial 2016). For instance, an effective methylene blue removal procedure
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1319

Fig. 8. (a) Schematic diagram of a fixed bed column filling with cellulose nanocrystal-alginate hydrogel developed from a previous batch adsorption study for effective methylene blue dye
removal (Adapted with permission from Mohammed et al. (2018)). (b) Schematic hierarchical structure of cellulose based nanofibrous ultrafiltration membrane consisted of three layers
of fibres in different diameters (Adapted with permission from Ma et al. (2018)).

was successfully established by incorporated recyclable cellulose elution of methanol/acetone/sodium hydroxide treatment (Beyki
nanocrystals-alginate hydrogel beads into a fixed bed filtration column, et al., 2016).
which a maximum adsorption capacity of 255.5 mg/g was recorded In the following, we attempted to cover several recent studies on
(Fig. 8a, Mohammed et al., 2016). This was generally in agreement nanocellulose products which may be helpful for future development.
with their previous Langmuir batch adsorption study (256.41 mg/g), Native celluloses are biopolymers posturing one methylol and two hy-
that also suggested a possibility of excellent reusability of at least five droxyl groups on each repeating unit, can be sophisticatedly modified
adsorption-desorption cycles with approximately 97% removal effi- and crosslinked into polymeric matrix to modulate water uptake capac-
ciency (Mohammed et al., 2015). In addition, it worth referring the fol- ity. Hsiao and his group attempted a novel class of multilayer cellulose
lowing studies regarding adsorbent regeneration and reusability: A based nanofibrous composite for an ultrafiltration membrane to sepa-
nanocellulose hybrid adsorbent up to four consecutive recycling cycles rate emulsified oil from a liquid mixture (Ma et al., 2010, 2012). The per-
after treating with hydrochloric acid/ethanol (1:1) mixture (Hussein meation flux of the said ultrafiltration membrane was significantly
et al., 2018), a hairy nanocellulose aerogel with at least six consecutive higher (above 10 times) than commercial ultrafiltration membrane
cycles via hydrochloric acid sodium hydroxide-ethanol procedure (i.e. PAN10 and PAN400, Sepro) with similar rejection ratio, attributed
(Yang and van de Ven, 2016), and lastly the magnetic-nanocellulose to the well electrospun of small diameter fiber in narrow size distribu-
polymeric ionic liquid with at least three consecutive cycles after fast tion (Fig. 8b). Melo et al. (2018) successfully incorporated cellulose
1320 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

Fig. 9. (a) SEM image of irregular surface with interconnected pores captured from cellulose composite (Adapted with permission from Melo et al. (2018)); (b) Illustration of trinity
synergistic treatment of complex wastewater using a cellulose hydrated titanate-bismuth oxide membrane, (Adapted with permission from Xiong et al. (2018)); (c) SEM image, EDS
spectra and elemental mapping of cationic cellulose hydrogel for anionic dye adsorption (Adapted with permission from Kono et al. (2016)); (di-ii) top and cross-sectional view of
SEM image of cellulose nanosheet membranes (Adapted with permission from Zhou et al. (2014)); (ei-ii) SEM image of free cellulose fiber and cellulose fiber coated with nano-
magnetite ZnO particles (Adapted with permission from Hassan et al. (2017)); (fi-ii) Antibacterial ability of cobalt/cellulose nanocomposite against S. aureus ATCC 25923 in comparison
with cellulose control sample (Adapted with permission from Alahmadi et al. (2017)).

nanowhiskers (90% crystalline) into chitosan-g-poly(acrylic acid) com- removal study. This was agreeable with an earlier study for efficient
posite for methylene blue dye adsorption (Fig. 9a). It was suggested that oil removal from non-stabilised oil-water mixture via functionalized
with as low as 5 w/w% of cellulose nanowhiskers involved in the hydro- cellulose fiber networks (Paul et al., 2016). A similar performance
gel, the adsorption capacity could be greatly improved to 1968 mg/g. It could be also achieved by a layer of cellulose nanosheet with controlla-
was also showing that up to 75% of the adsorbed methylene blue could ble thickness of 80–220 nm (Fig. 9d, Zhou et al., 2014).
be recovered with a reusability of at least 5 consecutive adsorption/de- Nanocellulose network can be also functionalised with magnetic
sorption cycles in b2% of efficiency loss. On the contrary, Xiong et al. properties for advanced water treatment. Native nanocellulose particles
(2018) attempted to coat a layer of CNC hydrogel on a flexible could be functionalised with magnetite colloidal suspension in a facile
titanate bismuth oxide membrane for better handling of super intricate method (Jodeh et al., 2018; Noor et al., 2018). Hassan et al. (2017) pre-
wastewater (Fig. 9b). From the study, the cellulose hydrogel top layer pared a magnetic composite via hybridization of nano-magnetite zinc
showed excellent ability to block oil phase into the system, following oxide and cellulose acetate using electrospinning technique (Fig. 9e).
by TNFs-Bi2O3 sub-layer to effectively remove toxic ions such as Cs+, 64% of phenol sorption could be achieved after 2 h of mixing with
I−, Cu2+, SeO4 2−, Pb2+, SeO3 2−, Sr2+ and Br−. It is worth mentioning 0.1 g adsorbent at 5 ppm phenol initial concentration. Magnetic cellu-
that this multi-layer membrane presented controllable shape in wide lose network also showed great absorption potential on resorcinol
range of acid and alkali condition, as well as good recyclability with sim- (Ding et al., 2017), and could be further developed for antibacterial
ple post-processing treatment. Other successful studies worth for fur- property (Alahmadi et al., 2017) (Fig. 9f). In fact, it was rather flexible,
ther development including: cationic cellulose hydrogel for anionic interesting and show great potential to enhance the current develop-
dyes removal (Kono et al., 2016) (Fig. 9c); graphene oxide-cellulose ment of nanocellulose material in water application (Cai et al., 2017;
nanowhiskers hydrogel for cationic dyes removal (Soleimani et al., Huang et al., 2018; Jiao et al., 2018).
2018); and double network hydrogel from wasted cotton fabrics for
heavy metal removal (Ma et al., 2018) (Fig. 10a). (Fig. 10b)For the 3.3. Energy
first time, Cheng et al. (2017) developed a nanoporous membrane
using tunicate cellulose nanocrystal (TCNC) derived from marine re- Increasing energy consumption encouraged the development of
sources for highly efficiency oil-water separation that could be in the more sustainable energy technologies with reduced carbon footprint.
form of oil-in-water nanoemulsion or oil-in-water microemulsion Green energy had long been discussed, but high capital and mainte-
(Fig. 10b). The transparency of TCNC membrane derived from well con- nance cost has remained a question. Nanocellulose have shown great
trolled nanoscale arrangement of cellulose particles via self-assembling potential owing to their unique physical and chemical properties,
of chiral nematic architecture contributed to the final success of the aroused to be a promising candidate for design of renewable materials
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1321

Fig. 10. (ai-ii) Illustration of graphical and actual cellulose/polyarylamide double network hydrogel synthesis pathway (Adapted with permission from Ma et al., 2018); (bi-v) Optical,
polarized, SEM and TEM images of tunicate CNC membrane, and finally graphical illustration on its chiral nematic arrangement to membrane optical and physical performance
(Adapted with permission from Cheng et al. (2017)).

Fig. 11. Illustration of generic fabrication of conductive nanocellulose via coating and composite approach.
(Adapted with permission from Du et al. (2017)).
1322 K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326

based energy devices in a more environmental friendly manner. Al- due to its low density, higher mechanical flexibility etc., while several
though many advantages from nanocellulose were realised, it cannot challenges such as poor reaction control and processability remained
be directly used for device fabrication due to its non-conductive nature. technically challenging (Baker et al., 2017).
Therefore, it was often modified chemically or physically, leading a wide The conventional Li-ion batteries and supercapacitors pose signifi-
spectrum of discussion in energy sector in the recent years (Du et al., cant environmental hazards during its manufacture and disposal. With
2017; Muhd Julkapli and Bagheri, 2017). In this section, a brief discus- increasing demand over the unstable renewable energy supply (e.g.
sion over the use of nanocellulose in soft composite material was wind power and solar energy), the high frequency usage of energy stor-
discussed, particularly in the area of energy storage and energy age has created a big issue to the environment. Cellulose-based
conversion. electroactive composite can be fine-tuned to have more flexible struc-
A conductive cellulose matrix can be prepared by combining con- ture at nanoscale. They are less sensitive to mechanical, owing to the
ductive electroactive materials (such as metal oxide, graphene oxide high porosity structure coated (or blended) with electronic charge
and conducting polymer) with modified nanocellulose (Shi et al., transporting materials, making them a promising separator and elec-
2016; Shi et al., 2013). Du et al. (2017) suggested that nanocellulose trode materials in storage devices (Edberg et al., 2017; Shi et al., 2016;
can be made conductive via two major strategies as shown in Fig. 11. Shi et al., 2015). Edberg et al. (2017) developed a thick-film
For the first one, conductive materials can be coated on a variety of nanocellulose supercapacitor system supported by mixed conductive
nanocellulose substrate via different techniques such as electro- polymer (PEDOT:PPS) and lignosulfonate. It was realised that the spe-
spinning (Zhang et al., 2017a, 2017b) and solvent evaporation cific capacitance increased from 110 to 230 Fg−1 with addition of ligno-
(Meulendijks et al., 2017). Otherwise, the nanocellulose can be in situ sulfonate, and a successful 700 charge/discharge cycles with no
polymerised or blended with electroactive materials for fabrication of observed decrease of capacitance was achieved. This was mainly attrib-
matrix composite. Among several kinds of conductive materials i.e. con- uted by successfully solving the lignosulfonate diffusion problem by
ductive carbons (carbon nanotube, graphene oxide, etc.), conductive adding adequate lignosulfonate into electrolyte. Nanocellulose aerogel
metals (Ag, Cu, etc.) and conductive polymers (Polyaniline, polypyrrole, is a promising nanomaterial for supercapacitor. It holds large surface
poly(3,4-ethylenedioxythiophene), etc.) that had been widely applied, area derived from its highly porous structure that encouraged fast ions
the conductive polymers have attracted significant attention recently adsorption/desorption from electrode via redox reaction. It has much

Fig. 12. (ai-ii) SEM images of CNF aerogels with and without reduced graphene oxide-SnO2 (Adapted with permission from Tan et al. (2018)); (b) Illustration on nanocellulose
incorporation into graphene oxide capacitor electrode network (Adapted with permission from Wang et al. (2017)); (c) SEM images of pristine CNF aerogel bead and its cross-
sectional view (Adapted with permission from Erlandsson et al. (2016)); (d) Nanocellulose aerogel as electrolyte carrier membrane in a quantum dot-sensitized solar cell (Adapted
with permission from Borghei et al. (2018)).
K. Tan et al. / Science of the Total Environment 650 (2019) 1309–1326 1323

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