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Cellulose Nanocrystals in Sustainable Energy Systems

Raúl Calle-Gil, Elizabeth Castillo-Martínez,* and Javier Carretero-González*

Most of them do not contain costly and

The transition to low-carbon emitting technologies provokes an increasing unfriendly metals and are profuse all
demand in energy conversion and storage systems such as fuel cells, batteries, over the earth. These characteristics
and supercapacitors, and consequently, the need for their raw materials. The use are crucial for the scalability and world-
wide implementation of battery systems
of new chemistries from earth-abundant precursors instead of scarce, toxic, and
around the world.
nondegradable components existing in current systems must be a priority in Because energy-providing processes
future years. Cellulose is the most abundant biopolymer on earth. Their crystalline occur at the electrode/electrolyte interface
constituents designated as cellulose nanocrystals (CNC) have been studied as in these systems, the design and develop-
functional materials due to their excellent structural and chemical properties. This ment of the electrode and electrolyte mate-
rials from biopolymers must favor the
review covers a recent collection of works on innocuous CNC-based materials
creation of adapted structural and textural
with special attention to the fabrication methodologies of electrodes, electrolytes, properties on them. This fact will facilitate
membranes, and separators. The implementation of these CNC-derived materials the molecular contact of the electrode sur-
in sustainable energy conversion and storage systems is also discussed. face and chemical species such as the sol-
vent and the electrolyte´s ions. Besides, it
will enable facile electrochemical reactions
1. Introduction and extend the life-term of the energy storage systems. Biopoly-
mers such as polysaccharides (chitosan, cellulose, or starch)
Raw materials production is the main contributor to the and polypeptides (collagen, keratin, and silk) are the ultimate
energy cost and CO2 generation during the manufacturing source of organic-based materials from nature. Among these
of energy conversion and storage systems, such as solar cells, biopolymers, cellulose is the most abundant and one of the
fuel cells, batteries, and supercapacitors.[1,2] To minimize the most versatile. Furthermore, their rich surface chemistry and
cost and the environmental impact, abundant materials and high mechanical properties make it suitable for a wide range
low-carbon emitting manufacturing routes must replace of applications including advanced electrodes and electrolytes.[4]
the conventional ones. For instance, electrode and electro- Cellulose is a hierarchical assembly of different structural com-
lyte materials based on organic and polymeric compounds ponents, where the CNCs are the smallest ordered units (Figure
that might ultimately have been prepared or extracted from 1a).[5] Because of their unique properties, nanocellulose-based
renewable biomass appear to be one sustainable solution.[2,3] materials have also been explored to build flexible, robust, and
thin energy devices due to its nanosized nature.[6]
Nanocellulose refers to cellulosic or cellulosic-derived materials
R. Calle-Gil, E. Castillo-Martínez
Department of Inorganic Chemistry with at least one nanoscale dimension (<100 nm). There are three
Chemical Sciences Faculty main types of nanocellulose: i) cellulose nanocrystals (CNCs), also
Complutense University of Madrid called cellulose nanowhiskers (CNWs) or nanocrystalline cellulose
Madrid 28040, Spain (NCN); ii) cellulose nanofibrils (CNFs), also known as nanofibril-
E-mail: [email protected]
lated cellulose (NFC); and iii) bacterial cellulose (BC), also known
R. Calle-Gil
Micro Electrochemical Technologies S.L. as biocellulose.[7] They fundamentally differ in form, method of
Móstoles Tecnológico production and index of crystallinity as it is shown in Table 1.
Móstoles 28935, Spain The following sections of this review show recent studies
J. Carretero-González related to the use of neat, hybrid-based and carbonized derived
Department of Polymeric Nanomaterials and Biomaterials CNCs as electrode materials in energy storage and conversion
Institute of Polymer Science and Technology
devices such as batteries or supercapacitors. Besides, most of
ICTP-CSIC
Madrid 28006, Spain the conversion and storage electrochemical systems consist of
E-mail: [email protected] two electrodes in contact with an electrolyte solution and gener-
The ORCID identification number(s) for the author(s) of this article ally separated by a solid membrane or separator. So, we include
can be found under https://doi.org/10.1002/adsu.202100395. in our discussion the implementation of CNC in solid electro-
© 2022 The Authors. Advanced Sustainable Systems published by lytes and in separator materials too.
Wiley-VCH GmbH. This is an open access article under the terms of
the Creative Commons Attribution-NonCommercial-NoDerivs License,
which permits use and distribution in any medium, provided the original
work is properly cited, the use is non-commercial and no modifications 2. CNC General Properties
or adaptations are made.
CNC properties derive from their chemical composition, high
DOI: 10.1002/adsu.202100395 aspect ratio, and large amount of surface hydroxyl functional

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Figure 1. a) Schematic view of the hierarchical organization of cellulose in plants. b) Polymeric structure of cellulose chains showing intrachain
hydrogen bonds (dashed line).

groups, which can establish intra and inter molecular the structure is stabilized by two intramolecular hydrogen
interactions. bonds, which are responsible for their high mechanical
Some of the main properties of CNCs are strength.[8,13] The aggregation of the chains into crystals and
fibrils during the biosynthetic process occurs via intermolecular
• High mechanical strength as a result of the strong intramo-
forces such as van der Waals interactions and hydrogen bonds.
lecular interactions.
The different conformations of the AGU molecules give rise to
• Aqueous assembling ability caused by intermolecular inter-
the seven identified cellulose polymorphs, some found in algae,
actions that favors the creation of 3D ordered structures.
bacteria, and higher plants.[8,13]
• Tunable surface chemistry because of the large amount of
surface hydroxyl functional groups that can be chemically
modified.
2.2. CNC Liquid Assembling Property

2.1. CNC Structure The presence of a large amount of hydroxyl groups grants
CNCs with exceptional physical and chemical properties such
CNCs are made of β(1-4) connected chains of anhydro-­ as high mechanical strength, high surface area, and tunable
glucopyranose units (AGU) in which every AGU unit is cork- surface chemistry.[5,9,13] Chemical modifications of CNCs can
screwed 180° with respect to its neighbors (Figure 1b). Due to be classified into covalent and noncovalent modifications.
the chair conformation adopted by the anhydro-glucopyranose Covalent modifications include the characteristic reactivity
units, all the hydroxyl groups are in the equatorial plane thus of the hydroxyl group such as oxidation,[14,15] cationization,[16]

Table 1. Morphology, method of production and crystallinity index of cellulose nanoforms.

Cellulose nanoform Morphology Method of production Index of crystallinity Reference

CNC Rod-like particles Acid hydrolysis of wood cellulose 70–95% [8–10]
CNF Thread-like aggregates Mechanical disaggregation of wood cellulose — [9–11]
BC Thread-like aggregates forming hydrogels Biosynthetic routes 70–80% [10—12]

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Figure 2. Images of CNCs suspensions in a) Native EG b) EG75%:water25% c) EG45%:water45%, and d) water, at concentration range of
φCNCs = 2.0–6.2%. Adapted with permission.[30] Copyright 2020, Royal Society of Chemistry. e) Phase separation in suspensions of cellulose
nanocrystals A) Low surface charge-CNC; B) High surface charge-CNC in pure water at different CNC mass fractions w, as indicated on each
vial cap. Reproduced under terms of the CC-BY license.[31] Copyright 2016, The Authors, published by Frontiers in Materials. f ) Schematic
representation of CNC orientation in both the isotropic and anisotropic (chiral nematic) phases. Adapted with permission.[8] Copyright 2010,
American Chemical Society.

esterification,[17] and silylation.[18] On the other hand, nonco- 3. CNC Electrodes

valent modifications are typically performed via adsorption of
ionic[19] and nonionic[20,21] surfactants to control the dispers- CNC-based electrodes have been widely studied either via intro-
ibility of the CNCs and to modify their surface properties.[8,13] ducing conductive materials onto a CNC scaffold[32–34] or have
For instance, CNCs form isotropic suspensions in water at been carbonized to get a 3D carbon-based conductive mate-
concentrations below 4 wt% due to the repulsive electrostatic rial.[35] In this review, we have classified the CNC-based elec-
interactions, and they aggregate at concentrations above trodes in two main groups, which will be discussed below: CNC
15 wt% due to the attractive intramolecular interactions.[22–25] hybrid electrodes and carbonized CNC electrodes.
However, in the range 4–15 wt%, CNCs self-assemble into
chiral nematic liquid crystals to minimize the repulsion
caused by the electrostatic interactions without aggregation. 3.1. CNC-Based Hybrid Electrodes
Both, the pitch and the volume of the chiral nematic phase
can be controlled as they depend on the interactions of the In the last decades, many researchers have tackled the insulating
CNCs with the solvent, which can be modified by varying character of the CNCs by combining them with conductive
factors like the ionic strength of the suspension, or the CNC materials such as conducting polymers, metallic particles, or
concentration (Figure 2).[21,26] These chiral nematic struc- carbon-derived materials using different preparation methods
tures can be freeze-dried to obtain hierarchical porous carbon (Figure 3). Two major strategies have been followed to prepare
structures with high surface area, after annealed in inert CNC-conductive composites: i) coating the conductive mate-
atmosphere. As it will be shown in the following sections, rial layers onto the surface of CNC substrates and ii) mixing
these porous structures are ideal for the development of the conductive materials inside the CNC substrates via in situ
electrode materials for energy conversion and storage appli- polymerization or blending. The in situ polymerization con-
cations.[27–29] In fact, the hierarchical porous structures can sists on dispersing a monomer as a repetitive building-block
accommodate large strain without pulverization, providing a precursor of the conducting polymer into the CNC matrix and
good electronic contact and conduction during the reversible then adding an initiator to build the CNC-conductive polymer
charge and discharge processes. Besides, the electrolyte ions composite.[36–38] On the other hand, blending is a technique
will easily access the redox active centers inside the porous used to mix different materials to keep the properties of each of
structures enabling capacity values close to the theoretical them individually in the hybrid composite or to enhance them
ones even at high cycling rates. through synergistic effect.[39]

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Figure 3. Fabrication routes to nanocellulose based conductive hybrid materials.

3.1.1. CNC-Conductive Polymer Hybrid Electrodes 3.1.2. CNC-Conductive Carbon Hybrid Electrodes

Conjugated polymers, have been deeply studied for their Since carbon nanomaterials such as carbon nanotubes (CNTs),
applications in energy as electrochemical capacitors, sensors, graphene oxide (GO), or reduced GO (rGO) have excellent
solar cells, Organic light emitting diodes and fuel cell elec- conductive properties (108 and 105 S cm−1 for graphene[43] and
trodes.[7,40,41] Unfortunately, they suffer from low “solubility,” so graphite, respectively[44]) and are chemically stable in harsh
recent studies have tried to overcome these problems by com- environments thanks to their low reactivity,[45] they have been
bining them with CNC due to its superior mechanical proper- studied in combination with CNCs. Although carbon nano-
ties and improved dispersibility in aqueous solution. The most materials can be coated onto CNC substrates, the interaction
studied CNC-based composites include conducting polymers, between the coated layer and the biopolymer is usually weak
such as polypyrrole (PPy, 0.3–100 S cm−1), poly­aniline (PANI, and the composites normally suffer from layer fall off. In con-
0.01–5 S cm−1), polyacetylene (PA, 3–1000 S cm−1), poly­ trast, the blending method let entrap the conductive materials
thiophene (PTh, 2–150 S cm−1), poly(phenylenevynilene) (PPV, inside the matrix, increasing the amount of carbon in the final
0.001–100 S cm−1) and their derivatives.[41] In fact, several composite and thus the electrical conductivity.[39]
studies have managed to successfully combine CNC-based Most of the studies have focused on the understanding of the
materials with conducting polymers via in situ polymeriza- fundamental properties of the CNC-based composites so they
tion. Tkalya et al.[42] successfully lowered the percolation can be implemented in advanced applications. Valentini et al.[46]
threshold for electronic conduction down to values of 0.4 wt%. studied the effect of mixing CNC with GO on the surface on
PEDOT:PSS in poly(3,4-ethylenedioxythiophene)/poly(styrene- the electrical properties of pristine GO. The resulting com-
sulfonate)-based polystyrene (PEDOT:PSS-based PS) compos- posite showed enhanced electrical conductivity due to the excel-
ites by adding CNCs, which act as a template. Moreover, the lent dispersion of the GO layers on the CNC matrix. In other
composite achieved higher electronic conductivity (7 S cm−1) studies, Tang et al.[47] fabricated a ternary system including mul-
than the blend (6 S cm−1), retaining 70% of the pure PEDOT- tiwalled carbon nanotubes (MWCNTs) and GO via blending,
PSS conductivity (10 S cm−1). using CNCs as a binder for the GO/MWCNT nanocomposite.
Some polymers, such as PPy tend to aggregate and grow The resulting MWCNT/GO/CNC paper showed an excellent
localized onto the CNCs so they are hard to disperse. Wu conductivity (9 S cm−1) compared to a CNT/cellulose paper
et al.[36] achieved an improved dispersion of the PPy on the (6.7 S cm−1)[48] and to the MWCNT/CNC (6 S cm−1) and GO/
TEMPO-oxidized CNC/PPy (TEMPO-CNC/PPy) composites CNC (1 S cm−1) coated papers.
with the addition of high molecular weight polyvinylpyrro- Carbon/CNC composites have recently developed some
lidone (PVP) prior to the polymerization. As a result of the important applications in sensors and flexible devices. Wu
better dispersion of PPy, the PPy/PVP/CNC composite showed et al.[33] studied the addition of CNC as a template to a carbon
higher electronic conductivity (37 S cm−1 for PPy/PVP/CNC black (CB) 3D network on natural rubber (NR). The CB/CNC/
and 5 S cm−1 for PPy/CNC) and capacitance (322 F g−1 for PPy/ NR material showed a decrease in the electrical conductivity
PVP/CNC and 238 F g−1 for PPy/CNC at 0.01 V s−1). percolation threshold with respect to the CB/NR traditional

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composite (3 vol% CB for CB/CNC/NR and 7 vol% CB CB/ studies, Lui et al.[52] used CNC as templates to synthesize Fe3O4
NR) with a great enhancement of 12 orders of magnitude nanoparticles (Fe3O4-NPs) with increased stability in aqueous
in electrical conductivity (6.6 × 10−14 S m−1 for CB/NR and media via coprecipitation method. The prepared CNC/Fe3O4-
2.4 × 10−2 S m−1 for CB/CNC/NR at 5 vol% CB). Furthermore, NPs composite was then coated on a paper forming a conduc-
raising the CB loading up to 7.5 vol% CB, results in an elec- tive layer on its surface (27 mS m−1).
trical conductivity of 0.8 S m−1. An increase in tensile strength
(760%) was also observed due to the incorporation of the CNC
template. Later, Wu et al.[32] lowered the electrical conductivity 3.2. Carbonized CNC Electrodes
percolation threshold of the CB/CNC/NR composite to 1.6 vol%
CB and maintained the 12 orders of magnitude increase in High surface area porous carbon materials have traditionally
conductivity at the lower load of carbon (4.8 × 10−13 S m−1 for been prepared from nonrenewable derivatives such as petro-
CB/NR and 3.5 × 10−1 S m−1 for CB/CNC/NR at 3.7 vol% CB). leum or coal using different methods[53,54] like physical or
CNCs have thus shown their potential application with carbon chemical activation[55–60] or templating.[61,62] However, the fab-
nanomaterials to achieve cheaper materials (lower percolation rication routes involving these materials are nonsustainable
thresholds and better dispersibility) with increased mechanical and expensive.[63] In the last decades, more sustainable mate-
properties and flexibility. rials with small particle size and high surface areas, such as
CNC aerogels,[64–68] have been carbonized to produce low cost
3D high surface area porous carbon structures. Yang et al.[69]
3.1.3. CNC-Inorganic Particle Hybrid Electrodes prepared lightweight hybrid electron conducting carbon aero-
gels by using via a sol–gel process. In Yang´s work different
Metallic particles such as Cu usually exhibit higher conductivity chemically modified CNC led the formation of hybrid aerogels
values (105 S cm−1)[49] than graphitic particles (104 S cm−1),[50] containing polypyrrole (PPy-NFs), polypyrrole-coated carbon
what makes them interesting candidates for combining with nanotubes (PPy-CNTs), or spherical manganese dioxide nano-
nanocellulose matrixes to further prepare conductive paper- particles (MnO2-NPs) within the 3D CNC framework (Figure 4).
based electrode materials. Some of the preparation methods for These aerogels were tested in symmetric supercapacitor cells
the particles and the CNCs are coating, doping,[51] and coprecip- with saturated Na2SO4 aqueous electrolyte. All the systems pre-
itation[52] (Figure 3). In their studies, Hebeish et al.[34] prepared sented high areal capacitance values (3.3, 2.4, and 2.1 F cm−2
a CNC-polyacrylamide copolymer and used it as a precursor for for PPy-NF, PPy-CNT, and MnO2-NP respectively at a scan rate
the synthesis of homogeneous Cu nanoparticle (CuNP)-doped of 2 mV s−1) and high stability (84.2% for PPy-NF, 61.7% for
CNC/polyacrylamide composite. The incorporation of a slight PPy-CNT, and 92% for MnO2-NP after 2000 cycles) with cou-
amount of CuNPs (0.8 wt%) meant an increase of 5 orders lombic efficiencies over 94% during cycling for all the devices.
of magnitude in conductivity of the composite compared to Zhuo et al.[35] synthesized high surface area hierarchical porous
the undoped copolymer (1 × 10−5 S m−1 and 5.5 × 10−10 S m−1, carbon aerogels derived from cellulose via one step activation-
respectively). The as-prepared composite was then proposed as carbonization. The aerogel showed high specific capacitance
a promising candidate material for conductive textiles. In other (328 F g−1 at 0.5 A g−1) and cycling stability (specific capacitance

Figure 4. A) Schematic representation of the aerogel precursors, including functionalized CNCs and capacitive nanoparticles, which form the initial
suspension of cross-linked clusters. B) The sol–gel process used to prepare aerogels. C) Photograph of the final hybrid aerogels with diameters of
1.5 cm. D) Photograph emphasizing the lightweight nature of a hybrid aerogel resting on top of a feather. E) Schematic showing the fabrication of
symmetric supercapacitor cells in CR2032 type coin cell cases with two hybrid aerogels separated by a porous polyethylene membrane in saturated
Na2SO4 aqueous electrolyte. Reproduced with permission.[71] Copyright 2015, Wiley.

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retention of 96% after 5000 cycles). In other studies, Nguyen Traditionally, polyolefins such as polyethylene (PE) and poly-
et al.[70] synthesized a mesoporous chiral TiC film by com- propylene (PP) have been widely used as separators, especially
bining CNC with peroxotitanate and letting it order into a chiral for Lithium-ion batteries (LIBs), whereas Nafion is the most
nematic phase. Once carbonized, the as prepared composite widely used membrane in fuel cells such as direct methanol
showed excellent properties when tested as capacitor (210 F g−1 fuel cell (DMFC) or polymer electrolyte membrane fuel cell
at 5 mV s−1). (PEMFC). However, some drawbacks of traditional separators
Recent studies have shown the possibility of tailoring the include hydrophobicity, low porosity, low electrolyte wettability,
properties of carbon nanomaterials, such as their wettability and weak mechanical and thermal properties. On top of that,
or their conductivity, via substitution with heteroatoms like most of the traditional separators derive from fossil fuels and
nitrogen, phosphorous, or sulfur, among others.[7,72,73] In fact, are expensive. To improve the electrochemical response of the
nitrogen has lately gathered a lot of attention thanks to its energy storage and conversion devices and to lower their cost,
ability to enhance the capacitance of the materials by increasing traditional separators must be replaced with materials with
the redox pseudocapacitance.[73] With CNC, Cheng et al.[74] better intrinsic properties or ease of chemical tunability such as
fabricated a N/O codoped carbonized CNC/PANi electrode nanocellulose.[85]
(c-CNC/PANi). The electrode was tested in a Li-ion battery and Nanocellulose offers high mechanical strength and rich func-
showed excellent electrochemical properties. The c-CNC/PANi tionality of hydroxyl groups, which are well known for strong
electrode exhibited low charge transfer resistance (76.3 Ω) and hydrogen bonding and ease of chemical modification. The
almost double reversible capacity at 200 mA g−1 over 100 cycles hydrogen bonding groups in nanocellulose can act as a path
(470 mA h g−1) than pristine c-CNC (240 mA h g−1). Besides, for proton hopping. The addition of dopant, cross-linker, or
it presented a Coulombic efficiency of almost 100% after polymeric additives with functional groups to nanocellulose can
2000 cycles. further enhance its ionic conductivity.[86] Nevertheless, nanocel-
lulose separators suffer from two main drawbacks. First, their
moisture content at room temperature. LIBs are very sensitive
4. CNC Electrolytes to water content (20–50 ppm) because it accelerates the degra-
dation of lithium salts, such as LiPF6[87] and CNCs moisture
Electrolytes are one of the key components of batteries.[75] Dif- content is far way above (21.4% at 95% relative humidity[88]).
ferent polymers have been used in solid or gel electrolytes.[76–79] For this reason, for their application in LIBs separators are sub-
Solid polymer electrolyte (SPE) research in LIBs has focused on jected to thermal treatments in order to remove the water sur-
polyethylene oxide (PEO) and its derivatives due to their high plus.[89] Second, nanocellulose papers are usually too densely
stability voltage window during cycling,[80] their high solvation packed and hinder the ionic conductivity lowering the perfor-
properties, which facilitates the solubility of different metal- mance of the LIBs.[90] All considered, nanocellulose separators
salts,[75] and their high molecular chain mobility, which facili- entail an improvement against traditional polyolefin separa-
tates Li+ conductivity.[81] Nevertheless, some of these polymer tors, although they need to be tuned to get better porosity and
electrolyte materials suffer from lack of mechanical strength reduce the water content in them. Wei et al.[91] developed a flex-
due to the volumetric changes and cannot prevent metal den- ible CNC-based membrane for a Li-metal battery. The mem-
drite growth occurring during the charge and discharge cycles, brane was composed of MnS/carbon nanofibers supported
which provokes the failure of the battery. To enhance the onto CNCs (MnS@CNC/carbon nanofibers). It showed excel-
mechanical properties of SPEs, nanocellulose has lately been lent electrochemical properties compared with the commercial
investigated as building block for solid polymer and gel-like PP membrane. The as-prepared membrane showed higher
electrolytes. Samir et al.[82] prepared a weakly cross-linked CNC/ ionic conductivity (1.533 × 10−3 S cm−1) than the PP membrane
PEO electrolyte. The hybrid electrolyte presented similar ionic (0.546 × 10−3 S cm−1) and the battery achieved higher capacities
conductivity over a wide range of CNC loadings (up to 10 wt%) (148.2 mA h g−1 for the MnS@CNC/carbon nanofiber mem-
similar to highly cross-linked PEO electrolyte (10−5 S cm−1 at brane vs 129.4 mA h g−1 for the PP membrane). Besides, the
20 and 40 °C, respectively). In addition, the mechanical strength Li/Li symmetric batteries indicated that the flexible ordered
of the electrolyte increased over 100 times when filled with CNCs. MnS@CNC/carbon nanofibers membrane could effectively
inhibit the Li dendrite growth and enhance the cycling stability
preserving 83% of the capacity after 600 cycles (123.1 mA h g−1)
5. CNC Separators and high Coulombic efficiency (99%) (Figure 5).
Apart from this, nanocellulose is known to enhance the bar-
Separators (membranes) are one of the main components of rier properties and mechanical stability of the membranes,
electrochemical systems such as fuel cells and batteries. They which are an essential requirement of the PEMs. Hasani-
prevent battery failures caused by short-circuit problems by Sadrabadi et al.[92] combined CNCs with Nafion altering its
keeping both electrodes separated from each other and act as microstructure. This alteration enhanced the proton conduc-
bridges for the ion exchange between the electrolytes at both tivity (0.2 S cm−1 of Nafion-CNC vs 0.15 S cm−1 of recast Nafion
sides in fuel cells. The ionic conductivity has been proven to at 120 °C and 100% relative humidity) and suppressed the
significantly affect the ohmic polarization (IR drop) of the cell. methanol permeability (2.3 × 10−7 cm2 s−1 for Nafion-CNC vs
Due to their important role, separators must have excellent 2.1 × 10−6 cm2 s−1 for recast Nafion) with 5 wt% CNC. Besides,
electrochemical and chemical stability, good electrolyte wetta- the Nafion-CNC composite membrane exhibited higher power
bility, and good mechanical and thermal properties.[83,84] density (91 mW cm−2) compared to recast Nafion (47 mW cm−2)

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Figure 5. Schematic illustrations of a) The Li dendrite growth on the bare Li anode. b) The uniform Li deposition on the Li anode with the MnS@CNC/
carbon nanofibers interlayer; and c) The synergistic effect of MnS@CNC/carbon nanofibers interlayer toward Li ions. Reproduced with permission.[91]
Copyright 2021, Elsevier B.V.

when tested in a methanol-air fuel cell with 5 m methanol. for lithium-ion batteries and supercapacitors. The performance
In other studies, Xu et al.[93] synthesized an amino acid (AA) of these sustainable energy conversion and storage systems is
functionalized CNC composite (CNC-AA) using 5 different assessed based on the physical and chemical properties of the
amino acids: glycine (Gly), 5-amino-valeric acid (Val), L-serine CNC-derived materials.
(Ser), L-leucine (Leu), and L-asparagine (Asp). The as-prepared Undoubtedly, there are still challenges to overcome that
CNC-AA composite was mixed with sulfonated poly(sulphone) require research and a better understanding of CNCs proper-
(SPSF) resulting in a SPSF/CNC-AA PEM. Among these ties. Among the main ones: i) the need to create hierarchical
composites, SPSF/CNC-Ser (10 wt% Ser) showed the highest CNCs-carbon derived electrodes exhibiting millimeter thick
proton conductivity value (23 S m−1 at 80 °C) which is sig- and presenting a multiscale porosity. These CNC materials
nificantly higher than commercial Nafion (3.5 S m−1 at 60 °C would have a great potential in electrochemical systems where
and 70% relative humidity[94] and 9 S m−1 at 95 °C and 100% an optimum balance between gravimetric power and energy
relative humidity[95]). These composites also showed improved densities is required; ii) the control of the final crystal struc-
methanol barrier properties thanks to the hydrogen interac- ture in liquid CNC assemblies will be crucial to create novel
tions between the SO3H groups of the SPSF and the OH mesoporous carbon structures with novel or enhanced electro-
and NH2 groups of the CNC-AAs. The methanol permeability chemical properties; iii) the creation of single-ion CNC electro-
decreased as follows: SPSF (11.8 × 10−7 cm2 s−1) > SPSF/CNC- lytes will also be most likely a promising strategy to enhance
Ser > SPSF/CNC-Asp > SPSF/CNC-Leu > SPSF/CNC-Val > ion conductivity in free-standing solid polymer electrolytes and
SPSF/CNC-Gly. binders, along with their mechanical properties. For that, by
applying the right surface chemistry, the anion might be cova-
lently anchored to the polymer backbone of the nanocrystal.
6. Summary and Prospects This new class of ionic CNCs conducting “salts” might evidence
ion transport numbers close to the unity, excellent mechanical
Renewable and innocuous CNCs are suitable candidates for properties, and an electrochemical stability window stable
low-cost, advanced functional materials operating in sustainable at high voltage values; iv) biosynthetic alternatives will allow
batteries, supercapacitors, and fuel cells. Because of the specific the creation of advanced multifunctional CNC materials. For
chemical composition and intermolecular interactions, CNCs instance, the biological incorporation of exogenous molecules
exhibit high crystallinity. These properties are crucial to fabri- before the growth of the nanocellulose fiber by BC, will allow
cate CNC-based porous separators and reinforced solid electro- to creation of novel or superior properties in CNC composites.
lyte membranes exhibiting high mechanical strength. Besides, Nonetheless, CNCs have already demonstrated to be appli-
the transformation of CNCs into carbonaceous porous mate- cable in a wide range of low-cost devices with extraordinary
rials has allowed the creation of advanced electrode materials impact in the energy field. As a result, we deem that on top of

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the talked-of improvements of nanocellulose over conventional [19] D. Bondeson, K. Oksman, Compos. Interfaces 2007, 14, 617.
materials, the more organized structure of the CNCs and their [20] O. J. Rojas, G. A. Montero, Y. Habibi, J. Appl. Polym. Sci. 2009, 113,
chemical and structural versatility makes them suitable candi- 927.
dates to fabricate low-cost, advanced electrodes, and electrolyte [21] Z. Hu, E. D. Cranston, R. Ng, R. Pelton, Langmuir 2014, 30, 2684.
[22] J. Araki, S. Kuga, Langmuir 2001, 17, 4493.
materials with enhanced response.
[23] M. D. Xue, T. Kimura, J. F. Revol, D. G. Gray, Langmuir 1996, 12,
2076.
[24] X. M. Dong, D. G. Gray, Langmuir 1997, 13, 2404.
Acknowledgements [25] S. Beck-Candanedo, D. Viet, D. G. Gray, Cellulose 2006, 13, 629.
[26] M. Winter, R. J. Brodd, Chem. Rev. 2004, 104, 4245.
R.C.G. gratefully acknowledge the Community of Madrid (No. IND2019/ [27] K. E. Shopsowitz, W. Y. Hamad, M. J. MacLachlan, Angew. Chem.,
AMB-17083) and the Micro Electrochemical Technologies S.L. (B5Tec) Int. Ed. 2011, 50, 10991.
for financial support. E.C.M. acknowledges financial support through the [28] C. Largeot, C. Portet, J. Chmiola, P.-L. Taberna, Y. Gogotsi, P. Simon,
Spanish Ministry of Science and Innovation through the ANOKIB project
J. Am. Chem. Soc. 2008, 130, 2730.
(No. RTI2018-094550-A-I00). J.C.G. acknowledges support from the
[29] J.-H. Lee, S.-J. Park, Carbon 2020, 163, 1.
Spanish Ministry of Economy, Industry, and Competitiveness (MINECO)
[30] D. Attia, N. Cohen, G. Ochbaum, Y. Levi-Kalisman, R. Bitton,
through a Ramon y Cajal Fellowship (No. RYC-2015-17722).
R. Yerushalmi-Rozen, Soft Matter 2020, 16, 8444.
[31] C. Honorato-Rios, A. Kuhnhold, J. R. Bruckner, R. Dannert,
T. Schilling, J. P. F. Lagerwall, Front. Mater. 2016, 3, 21.
Conflict of Interest [32] X. Wu, C. Lu, Y. Han, Z. Zhou, G. Yuan, X. Zhang, Compos. Sci.
Technol. 2016, 124, 44.
The authors declare no conflict of interest. [33] X. Wu, C. Lu, X. Zhang, Z. Zhou, J. Mater. Chem. A 2015, 3, 13317.
[34] A. Hebeish, S. Farag, S. Sharaf, T. I. Shaheen, Cellulose 2014, 21,
3055.
Keywords [35] H. Zhuo, Y. Hu, X. Tong, L. Zhong, X. Peng, R. Sun, Ind. Crops Prod.
2016, 87, 229.
batteries, cellulose, energy, nanocrystals, supercapacitors, sustainability [36] X. Wu, J. Tang, Y. Duan, A. Yu, R. M. Berry, K. C. Tam, J. Mater.
Chem. A 2014, 2, 19268.
Received: October 13, 2021 [37] B. A. Bhanvase, S. H. Sonawane, Chem. Eng. Process: Process
Revised: December 17, 2021 Intensif. 2014, 85, 86.
Published online: January 14, 2022 [38] X. Zhang, X. Wu, C. Lu, Z. Zhou, ACS Sustainable Chem. Eng. 2015,
3, 675.
[39] H.-W. Liang, Q.-F. Guan, Z.- Zhu, L.-T. Song, H.-B. Yao, X. Lei,
S.-H. Yu, NPG Asia Mater. 2012, 4, e19.
[1] M. Philippot, G. Alvarez, E. Ayerbe, J. Van Mierlo, M. Messagie, [40] C. Li, H. Bai, G. Shi, Chem. Soc. Rev. 2009, 38, 2397.
Batteries 2019, 5, 23. [41] Y. Shi, L. Peng, Y. Ding, Y. Zhao, G. Yu, Chem. Soc. Rev. 2015, 44,
[2] J. M. Allwood, J. M. Cullen, With Both Eyes Open, UIT Cambridge 6684.
Ltd, Cambridge 2012. [42] E. Tkalya, M. Ghislandi, W. Thielemans, P. van der Schoot,
[3] P. Navalpotro, E. Castillo-Martínez, J. Carretero-González, G. de With, C. Koning, ACS Macro Lett. 2013, 2, 157.
Sustainable Energy Fuels 2021, 5, 310. [43] E. Lago, P. S. Toth, G. Pugliese, V. Pellegrini, F. Bonaccorso, RSC
[4] X. Du, Z. Zhang, W. Liu, Y. Deng, Nano Energy 2017, 35, 299. Adv. 2016, 6, 97931.
[5] A. Zaman, F. Huang, M. Jiang, W. Wei, Z. Zhou, Energy Built [44] H. O. Pierson, Handbook of Carbon, Graphite, Diamonds and
Environ. 2020, 1, 60. Fullerenes, Elsevier, New York 1993, p. 43.
[6] W. Chen, H. Yu, S.-Y. Lee, T. Wei, J. Li, Z. Fan, Chem. Soc. Rev. 2018, [45] A. Forner-Cuenca, F. R. Brushett, Curr. Opin. Electrochem. 2019, 18,
47, 2837. 113.
[7] J. Jose, V. Thomas, V. Vinod, R. Abraham, S. Abraham, J. Sci. Adv. [46] L. Valentini, M. Cardinali, E. Fortunati, L. Torre, J. M. Kenny, Mater.
Mater. Devices 2019, 4, 333. Lett. 2013, 105, 4.
[8] Y. Habibi, L. A. Lucia, O. J. Rojas, Chem. Rev. 2010, 110, 3479. [47] Y. Tang, Z. He, J. A. Mosseler, Y. Ni, Cellulose 2014, 21, 4569.
[9] K. J. De France, T. Hoare, E. D. Cranston, Chem. Mater. 2017, 29, 4609. [48] M. Imai, K. Akiyama, T. Tanaka, E. Sano, Compos. Sci. Technol. 2010,
[10] H. Golmohammadi, E. Morales-Narváez, T. Naghdi, A. Merkoçi, 70, 1564.
Chem. Mater. 2017, 29, 5426. [49] B. Lee, Y. Kim, S. Yang, I. Jeong, J. Moon, Curr. Appl. Phys. 2009, 9,
[11] D. Klemm, F. Kramer, S. Moritz, T. Lindström, M. Ankerfors, e157.
D. Gray, A. Dorris, Angew. Chem., Int. Ed. 2011, 50, 5438. [50] Y. Liu, D. R. Treadwell, M. R. Kannisto, B. L. Mueller, R. M. Laine,
[12] W. Hu, S. Chen, J. Yang, Z. Li, H. Wang, Carbohydr. Polym. 2014, 101, J. Am. Ceram. Soc. 1997, 80, 705.
1043. [51] Z.-Y. Wu, B.-C. Hu, P. Wu, H.-W. Liang, Z.-L. Yu, Y. Lin, Y.-R. Zheng,
[13] D. Klemm, B. Heublein, H.-P. Fink, A. Bohn, Angew. Chem., Int. Ed. Z. Li, S.-H. Yu, NPG Asia Mater 2016, 8, e288.
2005, 44, 3358. [52] K. Liu, J. Nasrallah, L. Chen, L. Huang, Y. Ni, Carbohydr. Polym.
[14] Y. Habibi, H. Chanzy, M. R. Vignon, Cellulose 2006, 13, 679. 2015, 126, 175.
[15] A. Isogai, T. Saito, H. Fukuzumi, Nanoscale 2011, 3, 71. [53] T. Lin, I.-W. Chen, F. Liu, C. Yang, H. Bi, F. Xu, F. Huang, Science
[16] M. Hasani, E. D. Cranston, G. Westman, D. G. Gray, Soft Matter 2015, 350, 1508.
2008, 4, 2238. [54] J. Lin, Z. Peng, Y. Liu, F. Ruiz-Zepeda, R. Ye, E. L. G. Samuel,
[17] H. Yuan, Y. Nishiyama, M. Wada, S. Kuga, Biomacromolecules 2006, M. J. Yacaman, B. I. Yakobson, J. M. Tour, Nat. Commun. 2014, 5,
7, 696. 5714.
[18] C. Goussé, H. Chanzy, G. Excoffier, L. Soubeyrand, E. Fleury, [55] K. S. Lakhi, D.-H. Park, K. Al-Bahily, W. Cha, B. Viswanathan,
Polymer 2002, 43, 2645. J.-H. Choy, A. Vinu, Chem. Soc. Rev. 2017, 46, 72.

Adv. Sustainable Syst. 2022, 6, 2100395 2100395 (8 of 10) © 2022 The Authors. Advanced Sustainable Systems published by Wiley-VCH GmbH
 23667486, 2022, 4, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/adsu.202100395 by Nat Prov Indonesia, Wiley Online Library on [06/01/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
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[56] A. Nakayama, K. Suzuki, T. Enoki, K. Koga, M. Endo, N. Shindo, [75] R. Guo, L. Zhang, Y. Lu, X. Zhang, D. Yang, J. Energy Chem. 2020,
Bull. Chem. Soc. Jpn. 1996, 69, 333. 51, 342.
[57] Z. Hashisho, M. J. Rood, S. Barot, J. Bernhard, Carbon 2009, 47, 1814. [76] M. Armand, Solid State Ionics 1983, 9, 745.
[58] M. E. Ramos, P. R. Bonelli, A. L. Cukierman, M. M. L. Ribeiro Car- [77] M. Armand, M. Duclot, P. Rigaud, Solid State Ionics 1981, 3–4, 429.
rott, P. J. M. Carrott, J. Hazard. Mater. 2010, 177, 175. [78] P. Liu, E. Sherman, A. Jacobsen, J. Power Sources 2009, 189, 646.
[59] D. L. Johnsen, Z. Zhang, H. Emamipour, Z. Yan, M. J. Rood, Carbon [79] D. F. Shriver, B. L. Papke, M. A. Ratner, R. Dupon, T. Wong,
2014, 76, 435. M. Brodwin, Solid State Ionics 1981, 5, 83.
[60] B.-J. Kim, S.-J. Park, J. Colloid Interface Sci. 2007, 315, 791. [80] J. W. Fergus, J. Power Sources 2010, 195, 4554.
[61] M. Li, Y. Zhang, X. Wang, W. Ahn, G. Jiang, K. Feng, G. Lui, Z. Chen, [81] H. Qin, K. Fu, Y. Zhang, Y. Ye, M. Song, Y. Kuang, S.-H. Jang,
Adv. Funct. Mater. 2016, 26, 8408. F. Jiang, L. Cui, Energy Storage Mater. 2020, 28, 293.
[62] W. Luo, T. Zhao, Y. Li, J. Wei, P. Xu, X. Li, Y. Wang, W. Zhang, [82] M. A. S. Azizi Samir, F. Alloin, J.-Y. Sanchez, A. Dufresne,
A. A. Elzatahry, A. Alghamdi, Y. Deng, L. Wang, W. Jiang, Y. Liu, Macromolecules 2004, 37, 4839.
B. Kong, D. Zhao, J. Am. Chem. Soc. 2016, 138, 12586. [83] G. Venugopal, J. Moore, J. Howard, S. Pendalwar, J. Power Sources
[63] W. Lu, T. Wang, X. He, K. Sun, Z. Huang, G. Tan, E. G. Eddings, 1999, 77, 34.
H. Adidharma, M. Fan, Clean. Eng. Technol. 2021, 4, 100109. [84] P. Arora, Z. (John) Zhang, Chem. Rev. 2004, 104, 4419.
[64] J. Cai, H. Niu, Z. Li, Y. Du, P. Cizek, Z. Xie, H. Xiong, T. Lin, ACS [85] S.-J. Chun, E.-S. Choi, E.-H. Lee, J. H. Kim, S.-Y. Lee, S.-Y. Lee,
Appl. Mater. Interfaces 2015, 7, 14946. J. Mater. Chem. 2012, 22, 16618.
[65] L. F. Chen, X. D. Zhang, H. W. Liang, M. Kong, Q. F. Guan, P. Chen, [86] J.-H. Kim, B. S. Shim, H. S. Kim, Y.-J. Lee, S.-K. Min, D. Jang,
Z. Y. Wu, S. H. Yu, ACS Nano 2012, 6, 7092. Z. Abas, J. Kim, Int. J. Precis. Eng. Manuf. Technol. 2015, 2, 197.
[66] L. Dai, D. W. Chang, J.-B. Baek, W. Lu, Small 2012, 8, 1130. [87] M. Schmidt, U. Heider, A. Kuehner, R. Oesten, M. Jungnitz,
[67] Z.-Y. Wu, C. Li, H.-W. Liang, J.-F. Chen, S.-H. Yu, Angew. Chem., Int. N. Ignat’ev, P. Sartori, J. Power Sources 2001, 97–98, 557.
Ed. 2013, 52, 2925. [88] X. Guo, Y. Wu, X. Xie, Sci. Rep. 2017, 7, 14207.
[68] L. Deng, R. J. Young, I. A. Kinloch, A. M. Abdelkader, S. M. Holmes, [89] A. G. Assaf, R. H. Haas, C. B. Purves, J. Am. Chem. Soc. 1944, 66,
D. A. De Haro-Del Rio, S. J. Eichhorn, ACS Appl. Mater. Interfaces 66.
2013, 5, 9983. [90] J.-H. Kim, J.-H. Kim, E.-S. Choi, H. K. Yu, J. H. Kim, Q. Wu,
[69] X. Yang, K. Shi, I. Zhitomirsky, E. D. Cranston, Adv. Mater. 2015, 27, S.-J. Chun, S.-Y. Lee, S.-Y. Lee, J. Power Sources 2013, 242, 533.
6104. [91] L. Wei, N. Deng, X. Wang, H. Zhao, J. Yan, Q. Yang, W. Kang,
[70] T.-D. Nguyen, E. Lizundia, M. Niederberger, W. Y. Hamad, B. Cheng, J. Membr. Sci. 2021, 637, 119615.
M. J. MacLachlan, Chem. Mater. 2019, 31, 2174. [92] M. M. Hasani-Sadrabadi, E. Dashtimoghadam, R. Nasseri,
[71] X. Yang, E. D. Cranston, Chem. Mater. 2014, 26, 6016. A. Karkhaneh, F. S. Majedi, N. Mokarram, P. Renaud, K. I. Jacob,
[72] D. Jana, C.-L. Sun, L.-C. Chen, K.-H. Chen, Prog. Mater. Sci. 2013, J. Mater. Chem. A 2014, 2, 11334.
58, 565. [93] X. Xu, G. Zhao, H. Wang, X. Li, X. Feng, B. Cheng, L. Shi, W. Kang,
[73] X. Y. Chen, C. Chen, Z. J. Zhang, D. H. Xie, X. Deng, Ind. Eng. Chem. X. Zhuang, Y. Yin, J. Power Sources 2019, 409, 123.
Res. 2013, 52, 10181. [94] R. Sigwadi, M. S. Dhlamini, T. Mokrani, F. Ṋ emavhola, P. F. Nonjola,
[74] M. Cheng, J. Xia, J. Hu, Q. Liu, T. Wei, Y. Ling, W. Li, B. Liu, ACS P. F. Msomi, Heliyon 2019, 5, e02240.
Appl. Energy Mater. 2021, 4, 9902. [95] H.-Y. Li, Y.-L. Liu, J. Mater. Chem. A 2014, 2, 3783.

Raúl Calle Gil graduated in Chemistry and holds a Master’s degree in Biochemistry, Molecular
Biology, and Biomedicine from the Universidad Complutense de Madrid. He is currently a Ph.D.
candidate in Advanced Chemistry at the Universidad Complutense de Madrid in collaboration
with Micro Electrochemical Technologies S.L. His research focuses on the development of
sustainable electrode materials from abundant biopolymers, and their application in advanced
energy storage and conversion systems.

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Elizabeth Castillo Martínez did her Ph.D. in Solid State Chemistry at Universidad Complutense de
Madrid in 2008. After postdoctoral stays at Alan G. MacDiarmid NanoTech Institute in Texas, CIC
energiGUNE, and the University of Cambridge she is currently professor in Inorganic Chemistry
at Universidad Complutense de Madrid. Her research is focused on the development and
understanding of electrode materials for energy storage applications, such as lithium, sodium,
and potassium ion batteries.

Javier Carretero-Gonzalez is a tenured scientist at the Polymer Science and Technology Institute
of the Spanish Research Council. He is currently working on new functional materials for
sustainable energy applications, along with the implementation of advanced characterization
tools for understanding the operation mechanisms in these energy materials systems. He holds
a bachelor´s degree in chemistry from Universidad Complutense de Madrid (2002) and a Ph.D.
degree in science from Universidad Nacional de Educación a Distancia (2009).

Adv. Sustainable Syst. 2022, 6, 2100395 2100395 (10 of 10) © 2022 The Authors. Advanced Sustainable Systems published by Wiley-VCH GmbH