Wood-Based Nanotechnologies Toward Sustainability

REVIEW
Sustainable Nanomaterials www.advmat.de
Wood-Based Nanotechnologies toward Sustainability

Feng Jiang, Tian Li, Yiju Li, Ying Zhang, Amy Gong,* Jiaqi Dai, Emily Hitz, Wei Luo,*
and Liangbing Hu*
to alleviate our reliance on petroleum-based

With over 30% global land coverage, the forest is one of nature’s most gen- materials. Beyond abundance and biodeg-
erous gifts to human beings, providing shelters and materials for all living radability, wood is also a carbon-neutral
beings. Apart from being sustainable, renewable, and biodegradable, wood material that does not contribute net CO2
and its derivative materials are also extremely fascinating from a mate- increase due to the cyclic carbon fixation
during photosynthesis and release during
rials aspect, with numerous advantages including porous and hierarchical
degradation. Given these advantages, wood
structure, excellent mechanical performance, and versatile chemistry. Here, has been considered as a potential replace-
strategies for designing novel wood-based materials via advanced nano- ment for petroleum-based materials to sup-
technologies are summarized, including both the controllable bottom-up port continued sustainable growth.
assembly from the highly crystalline nanocellulose building block and the Throughout history, wood has been
the primary material for tools, buildings,
more efficient top-down approaches directly from wood. Beyond material
and fuels that support human activity.
design, recent advances regarding the sustainable applications of these novel However, the functions of wood have
wood-based materials are also presented, focusing on areas that are tradition- been limited by its intrinsic properties
ally dominated by man-made nonrenewable materials such as plastic, glass, including bulkiness, low mechanical
and metals, as well as more advanced applications in the areas of energy properties, nontransparency, and noncon-
storage, wastewater treatment and solar-steam-assisted desalination. With all ductivity. Therefore, it has been gradu-
ally replaced by other materials, such as
recent progress pertaining to materials’ design and sustainable applications
synthetic polymers, glass, and metals.
presented, a vision for the future engineering of wood-based materials to pro- With the advancement of nanotechnology,
mote continuous and healthy progress toward true sustainability is outlined. nanomaterials derived from wood have
been successfully synthesized and are well
suited to expand its application to more
1. Introduction emerging areas such as the environment, energy, and biomedi-
cine. Therefore, given the rapid expansion of bio-based nano-
With the ever-increasing world population and continuous technologies and the stringent demands for sustainable devel-
depletion of the fossil fuel reserves, as well as the anthropo- opment, it is pressing to revisit wood-based materials as sus-
genic environmental deterioration that includes water, soil and tainable sources to satisfy our continuous needs, alleviating our
air pollution, climate change, and nondegradable solid waste, fear of the depletion of nonrenewable natural resources.
tremendous interest has been drawn to sustainable develop- Here, we cover the most recent advances in designing hier-
ment. Sustainable materials, especially those derived from trees archical structures using wood and wood-based nanomaterials,
and other renewable and biodegradable lignocellulosic biomass, including both the bottom-up assembly from nanocellulose
should be given high-priority consideration as part of the solution into varied 1D, 2D, and 3D forms and the recently developed
top-down approaches that introduce novel functionalities to
existing wood hierarchical structures. Progress in the applica-
Dr. F. Jiang, T. Li, Y. Li, Y. Zhang, Dr. A. Gong, J. Dai, E. Hitz, W. Luo,[+]
Prof. L. Hu
tion of these hierarchical structures to emerging sustainable
Department of Materials Science and Engineering areas will be reviewed to emphasize how these traditional
University of Maryland College Park woody materials, now transformed by nanotechnologies,
College Park, MD 20742, USA may be used to improve the sustainability of biodegradable
E-mail: amysgong@umd.edu, amysgong@gmail.com; flexible electronics, natural energy harvesting, thermal regu-
weiluo@tongji.edu.cn; binghu@umd.edu
lation in green buildings, sustainable energy storage, envi-
Dr. A. Gong
Inventwood ronmental remediation, and efficient solar steam generation
LLC toward desalination. To date, several very important reviews on
Hyattsville, MD 20782, USA the structures and applications of wood- and cellulose-based
The ORCID identification number(s) for the author(s) of this article materials have been published, and due to the limited space
can be found under https://doi.org/10.1002/adma.201703453. available here, inclusion of comprehensive knowledge on all
[+]Presentaddress: Institute of New Energy for Vehicles, School of these aspects is infeasible. For more detailed reviews on each
Materials Science and Engineering, Tongji University, Shanghai aspect, the readers will be directed to other more compre-
201804, China hensive or specific reviews.[1–7] The primary focus here will
DOI: 10.1002/adma.201703453 be placed on how these bio-based materials could potentially
Adv. Mater. 2017, 1703453 1703453 (1 of 39) © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.advmat.de
replace nondegradable plastic, glass, and metal in electronics,

energy storage, constructions, water treatments, and other Feng Jiang received his
environmental remediation. Despite their attractive qualities, B.S. (2004) and M.S. (2007)
bio-based alternatives are still far from actualizing society’s degrees in wood science and
push for complete sustainability, in particular due to (1) infe- technology from Northwest
rior performance of the wood-based materials compared to A&F University (China) and
synthetic counterparts, (2) economic drawbacks of the high Chinese Academy of Forestry,
production cost of wood-based materials, and (3) secondary respectively. He got his
contamination of the environment through treatment and Ph.D. degree in macromo-
functionalization of wood-based materials to preventing total lecular science and engi-
sustainability. Nevertheless, we are on track toward sustain- neering from Virginia Tech in
ability, and ultimate success will not only depend on techno- 2011. From 2011 to 2016, he
logical breakthroughs, but also on the collective contributions received postdoctoral training
of social scientists and politicians. at the University of California Davis. Currently, he is a
postdoctoral researcher in Prof. Liangbing Hu’s group at
University of Maryland, and will be an Assistant Professor
at University of British Columbia. His research focuses on
2. Hierarchical Mesostructures from
sustainable functional biomaterials, including bio-based
Wood-Based Nanomaterials nanomaterials isolation, modification, characterization,
Wood, as shown in Figure 1, has naturally evolved to have a and assembly, as well as their advanced applications in
hierarchical structure that spans multiple orders of magnitudes energy and environmental areas.
in dimensions, serving different functionalities at each length
scale to support tree growth and provide materials for human Amy Gong received her B.S.
use. The tens of meters long trunk uplifts the tree crowns for in chemical and materials
more sunlight, an essential factor for photosynthesis, and also engineering from National
provides building materials for protection from the elements. Central University in 2006.
Down to the millimeter and micrometer range, the structure She received her Ph.D. in
of wood varies significantly for different types of trees, gener- chemical and environmental
ally classified as gymnosperms and angiosperms. The primary engineering at UCR with
cells in gymnosperms are called tracheids of ≈2–4 mm in length Sharon Walker in 2011. She
and 20–40 µm in diameter, which provide mechanical strength is a post-doctoral associate
and serve as conduits for water and nutrient transport.[8] More at University of Maryland,
complicated cells can be found in angiosperms that include College Park (UMCP) working
the 0.3–0.6 mm long and 30–130 µm wide vessels for water with Liangbing Hu. Her
and nutrient transport, as well as the 0.8–1.6 mm long and research interests include transparent paper, hazy trans-
14–40 µm wide libriform cells for mechanical support. These parent wood, water purification, and microbial fuel cells.
cells have found widespread application in papermaking, espe- She is also the co-founder and CEO of Inventwood LLC.,
cially for those in gymnosperms due to the higher aspect ratio. which is a Maryland registered start-up to commercialize
All plant cells have cell walls consisting of compounds including wood-related technology to increase energy efficiencies in
cellulose, hemicelluloses, and lignin, with different composi- buildings, and realize low-cost water-purification devices.
tions varying by species. At this nanometer scale, the elemen-
tary cellulose fibrils bind into 10–20 nm microfibrils, which
Liangbing Hu is an associate
pack in parallel with each other primarily in the S2 layer of the
professor at University of
secondary cell wall at different angles along the axis direction.[9]
Maryland College Park. His
These aligned cellulose microfibrils are responsible for mechan-
research interests include
ical support of the cell walls; strong correlations have been found
nanomaterials and nanostruc-
to exist between the microfibril angles and stiffness.[10] Within
tures, roll-to-roll nanomanu-
the 1.5–3.5 nm elementary fibrils, individual cellulose chains
facturing, energy storage
assemble with each other to form ordered or crystalline regions
focusing on solid-state bat-
interspersed with disordered or amorphous regions. The sizes of
teries and Na ion batteries,
crystalline regions in native cellulose are usually in the order of
and printed electronics. He is
100–250 nm long and 3–10 nm wide, which, through nanotech-
the (founding) director of the
nology, can be isolated as individual crystallites.[4,8] Therefore,
Center for Advanced Paper
wood can be considered a naturally occurring nanocomposite
and Textile (CAPT) at the University of Maryland College
with highly crystalline cellulose elementary fibrils glued together
Park (www.capt.umd.edu). He is also the co-founder of
by the interfibril compounds of hemicellulose and lignin.
Inventwood, Inc. with efforts to further commercialize
Due to the sophisticated assembly of these lignocellulosic
nanocellulose-based nanotechnologies.
nanomaterials by nature, wood has excelled in many aspects
over man-made nonrenewable materials, especially in the
Figure 1. Schematics of the hierarchical structures of trees showing macro- to nanoscale dimensions, and their advanced applications via sustainable
nanotechnologies.
traditional areas of building, furniture, and packaging. It is cellulose microfibrils of 25–30 nm wide, with a deposited outer
envisioned that, by further functionalizing and engineering lignin layer to strengthen the cell wall structure.[16]
these nature-based nanomaterials using newly developed nano- To access and make use of the microfibrils and sub-microfi-
technologies, advanced materials with properties that surpass brils, their interfibril lignin and hemicellulose can be removed
traditional wood can be developed. through mechanical defibrillation, yielding what is called
In this section, recent advances in designing hierarchical “microfibrillated cellulose.”[17] However, isolation of the 3–4 nm
structures from wood and wood-based nanomaterials via dif- wide elementary fibrils is more challenging owing to the strong
ferent strategies will be summarized, including both the con- interfibril hydrogen bonding, thus requiring more extensive
trolled assembly of the basic nanocellulose building blocks into chemical or biological treatment, as well as aided by mechan-
hierarchical 1D, 2D, and 3D structures, as well as engineering ical shearing, to disrupt the interfibril hydrogen bonding. Iso-
wood nanocomposites via top-down chemical and mechanical lation of elementary fibrils is possible through various acces-
processes to endow novel properties that are normally not pre- sible surfaces including (A) highly crystalline surface chains,
sented in traditional wood materials. (B) disrupted surface chains at the crystalline regions, and
(C) strain-distorted regions of tilt and twist (Figure 2b).[18] These
regions are all weak points that are susceptible to chemical or
2.1. Multifunctional Mesostructures by Bottom-Up mechanical treatment, liberating individual elementary fibrils
Assembly of Nanocellulose from cellulose microfibrils.
Acid hydrolysis of wood cellulose fibers primarily degrades
In the wood cell walls, cellulose biosynthesis is accomplished the amorphous regions between crystallites, generating rigid
through multiple cellulose synthase subunits according to Pres- rod-like cellulose nanocrystals (CNCs). Sulfuric acid has
ton’s “ordered granule hypothesis,”[11] called terminal complexes been commonly used to generate highly uniform CNCs of
(TCs). Each rosette-shaped TC consists of six subunits, which ≈100–300 nm long and 3–5 nm wide from wood cellulose pulp
contains a hexamer of cellulose synthase enzyme (CeSA) to poly (Figure 2c).[19] However, sulfuric acid hydrolysis also leads to an
merize glucan chains at the nonreducing end.[12,13] The 25–30 nm esterification reaction on the surface hydroxyls, forming sul-
wide rosette TCs are guided by the microtubules to float in the fate hemiester groups that are found to be detrimental to the
plasma membrane, leading to the orientation of cellulose chains thermal stability of CNCs.[20] Therefore, other types of acids
in the cell walls.[14] A total of 36 glucan chains can be extruded such as hydrochloric,[21] phosphoric,[22] phosphotungstic,[23] and
and bound with each other to form the cellulose elementary organic acids[24] have also been explored to generate more ther-
fibrils, reaching ≈3.5 nm in higher plants (Figure 2a).[13,15] It has mally stable CNCs. Besides, due to the preferential hydrolysis
been proposed that 16–20 elementary fibrils are closely packed of amorphous regions to soluble products that are impossible
with each other to form fibrils of 12 nm wide, among which to recover, acid hydrolysis generally leads to low yields of less
hemicellulose is deposited; together, these structures are respon- than 30% but very high crystallinity approaching 90%.[25]
sible for water transport within cell walls. Additionally, four of As an alternative to CNCs, cellulose nanofibrils (CNFs)
these separated fibrils can further assemble into the so-called are isolated from cellulose fibers by breaking the interfibril
Figure 2. Hierarchical structure of cellulose microfibrils and elementary fibrils. a) Cross-sectional model of the ultrastructural organization of cell wall
components in wood, showing the assembly of elementary fibrils into microfibrils. Reproduced with permission.[16] Copyright 1971, John Wiley & Sons.
b) Schematic of the elementary fibrils to illustrate the accessible surface of (A) coalesced surfaces of high order, (B) readily accessible slightly disordered
surfaces, and (C) readily accessible surfaces of strain-distorted tilt and twist regions. Reproduced with permission.[18] Copyright 1971, John Wiley & Sons.
c) TEM image of wood cellulose nanocrystals (CNCs). Reproduced with permission.[1] Copyright 2011, The Royal Society of Chemistry. d) TEM image
of cellulose nanofibrils (CNFs). Reproduced with permission.[27] Copyright 2007, American Chemical Society. e) HRTEM image of wood–cellulose
nanofibrils showing the crystalline lattice structure. Reproduced with permission.[28] Copyright 2015, National Academy of Science.
hydrogen bonding, leading to long and flexible nanofibrils that 2.1.1. 1D Macrofibers
resemble the individual elementary fibrils in cell walls. Disrup-
tion of these interfibril hydrogen bonding can be aided with 1D continuous cellulose macrofibers are heavily employed in
chemical[6] and enzymatic[26] treatment to reduce the energy many areas including textiles, filtration, construction, and rein-
consumption during defibrillation. 2,2,6,6-tetramethylpiperi- forced composites. Nowadays, except for cotton fibers, most
dine-1-oxyl (TEMPO) radical oxidation selectively converts the of the cellulose fibers (such as viscose, Rayon, and Lyocell)
surface primary hydroxyls in the accessible regions into car- are produced via regeneration processes. Cellulose regenera-
boxyl groups, facilitating isolation of highly uniform cellulose tion requires heavy chemical doses and destroys the naturally
nanofibrils of 3–4 nm wide and up to several micrometers long occurring cellulose I crystalline structure,[48] resulting in infe-
(Figure 2d). High-resolution transmission electron microscopy rior mechanical properties. Given that, the ability to assemble
(HRTEM) imaging of the cellulose nanofibrils clearly shows these naturally occurring cellulose nanofibrils into macrofibers
the crystalline lattice structure that contributes to its excel- has attracted much interest due to reduced chemical input and
lent mechanical properties.[28] The isolation and characteris- preservation of the native cellulose I crystalline structure.
tics of nanocellulose have been well documented in previous All-cellulose macrofibers assembled from cellulose nanofi-
reviews[3–6,29] and will not be recounted here. brils were first reported in 2011, which were achieved by
As the basic building blocks for wood cell wall structure, the extruding an aqueous suspension of nanocellulose into coagula-
cellulose elementary fibrils demonstrate numerous advantages tion solvents, such as acetone, ethanol, dioxane, and tetrahydro-
such as superb mechanical properties of 120–220 GPa for Young’s furan (Figure 3a).[34,35] The contact of extruded viscose cellulose
modulus[1,30] and 1.6–3 GPa for the strength,[31] low thermal nanofibril suspensions with a coagulation solvent leads to the
expansion coefficient of 10−7 K−1,[32] and super high optical transformation of a hard skin at the outer surfaces, which gradually
parency.[1,33] Therefore, it has attracted tremendous interest in penetrates into to the center via solvent exchange to solidify the
transferring these excellent characteristics from the nanoscale fiber structures. The solidified macrofibers show birefringence
to the macroscale, through bottom-up assembly of nanocellulose under cross polarizers (Figure 3b), indicating preferred align-
building blocks, with assembled macroscopic forms including ment of the cellulose nanofibrils induced by shearing forces,
1D fibers or filaments,[34–37] 2D films and papers,[38–41] as well as as also being observed from the scanning electron microscope
3D hydrogels[42] and aerogels,[43–47] which have opened up more (SEM) image (Figure 3c). Details on the strategies in improving
opportunities for advanced applications (Figure 3). the mechanical properties of nanocellulose macrofilament will
Figure 3. Assembled hierarchical structures using nanocellulose as building blocks, 1D macrofibers, and macrofilaments. a) Photograph of a 1 m long
macrofiber of ≈0.2 mm diameter from cellulose nanofibrils. Reproduced with permission.[35] Copyright 2011, WILEY-VCH. b) Optical micrography image
of CNF 2% filament between crossed polarizers. Reproduced with permission.[49] Copyright 2016. c) Scanning electron microscope (SEM) image of
cellulose nanofibrils filament. Reproduced with permission.[37] Copyright 2014, Macmillan Publishers Limited. 2D transparent papers: d) Super-clear
nanopaper from CNCs. Reproduced with permission.[50] Copyright 2017, WILEY-VCH. e) Photograph of the light scattering effect of transparent paper
with laser passing though. Reproduced with permission.[51] Copyright 2013, American Chemical Society. f) Atomic force microscopy (AFM) phase
image of transparent nanopaper from CNCs. Reproduced with permission.[50] Copyright 2017, WILEY-VCH. 3D aerogels, g) photograph of a cellulose
nanofibrils aerogel standing on top of a dandelion. h) SEM image of a cellulose nanofibril aerogel showing highly porous honeycomb structures.
g,h) Reproduced with permission.[43] Copyright 2014, the Royal Society and Chemistry. i) Photograph of a transparent liquid crystalline nanocellulose
aerogel. Reproduced with permission.[51] Copyright 2014, WILEY-VCH.
be reviewed in the following section on sustainable applications or optoelectronics. Therefore, to advance the applications
for super strong materials. of these biodegradable substrates in emerging electronic
Besides wet spinning, dry spinning has also been reported to areas, with intention to replace the commonly used petro-
directly spin-concentrate cellulose nanofibril aqueous suspen- leum-based plastic substrate, >90% transparency nanopaper
sion followed by drying in air, showing good mechanical prop- matching the superior optical clarity of plastic has been devel-
erties of 222 MPa for tensile strength and 12.6 GPa for Young’s oped (Figure 3d,f).[33] Super-clear transparent nanopaper can
modulus.[52] Given that no coagulation solvent is used, the dry- be prepared by compacting the 3–4 nm wide TEMPO-oxidized
spinning process is much greener than the wet-spinning and is cellulose nanofibrils (TOCNFs). The resulting film had a
more scalable. high transmittance of 90% at 600 nm, density ranging from
1.45 to 1.46 g cm−3,[39] and excellent oxygen barrier perfor-
mance, indicating the lack of large interfibril pores to scatter
2.1.2. 2D Films light.[40,53]
More appealing, the transparent nanopaper demonstrates
Conventional paper, due to the overlaid large cellulose fibers better light management than plastic substrates by showing
and permeation of air pockets among these fibers, strongly both high transparency and tunable haze, which have found
scatters incident light due to the mismatch of the refractive more applications where both light transmittance and scat-
indices between cellulose (1.5) and air (1), and therefore tering are desired such as thin-film solar cells.[41] Several
appears opaque.[38] Along with the opacity, the high rough- different strategies have been employed to tune the haze
ness and strong water wicking properties of the conventional of transparent nanopapers. TEMPO oxidation of cellulose
paper make it less ideal for applications in printed electronics fibers has been found to reduce fiber length and increase the
amount of fine strands (fibers with length less than 200 µm), 2.1.3. 3D Aerogels
as well as to crush and unzip the fibers in the axial direc-
tion, which all contribute the formation of denser films with Beyond 1D macrofibers and 2D transparent nanopapers, nano-
high optical transmittance of over 90%.[54] Owing to the large cellulose has also been assembled into 3D aerogels, showing
fiber diameter of ≈26 µm, this transparent film made from numerous promising characteristics of low density, high
TEMPO-oxidized fibers also demonstrated a high optical haze porosity, high specific surface area, flexibility, and tunable
of ≈60%, in significant contrast to the super-clear transparent surface chemistry.[60] Cellulose nanofibrils, owing to the high
nanopapers made from cellulose nanofibrils.[33,54] By further aspect ratios and prevalent surface polar groups, have been
regulating the weight ratios of microsized TEMPO-oxidized found to form robust network structures through interfibril
fibers to the cellulose nanofibril after homogenization, the hydrogen bonding via a simple freezing–thawing process.[45]
transmission haze varies from 20% to 60%, with unchanged Aerogel with an ultralow density of ≈1 mg cm−3 and ultrahigh
≈90% transmittance.[41] By stretching the films fabricated porosity of ≈99.9% can be facilely prepared by simply lowering
from cellulose nanofibrils grafted with poly(ethylene glycol) the suspension concentration (Figure 3g).[43] Extensive associa-
(PEG), wrinkles with wavelength ranging from 500 nm to tion among the individual cellulose nanofibrils is observed from
1 µm are found to be present parallel to the axis of stretching, the honeycomb structure of the aerogel (Figure 3h), showing
which induce more light scattering and hazy phenomena due all-cellulose nanofibrils are closely assembled with each other
to the increased surface roughness.[55] It is also found that forming an intact film. Besides, the fact that CNF can form a
the dispersion solvent can affect the transmission haze of the strong hydrogel through a freezing–thawing process opens up
nanopaper; it showed that the haze increased from 4.2% to more possibilities for surface modification normally carried
49.3% to 90.1% by gradually increasing the ratio of ethanol out in solvents that are incompatible with cellulose. This idea
from 0% to 50%, and 90%, respectively, for the same cellu- has been tested by crosslinking the CNF hydrogel with meth-
lose nanofibrils with a similar total transmittance of ≈90%.[56] ylene diphenyl diisocyanate in acetone, showing simultaneous
This tunable haze is due to the inhomogeneous dispersion improvement in mechanical properties, surface hydrophobicity,
of cellulose nanofibrils in a mixed ethanol/water suspension specific surface area, and thermal stability.[44]
that leaves numerous trapped air voids after drying, which Due to the high porosity and presence of numerous air
are confirmed by the decreasing packing density from 1.48, to pockets in the nanocellulose aerogel, it commonly presents
1.15, to 0.81 g cm−3. as a white and opaque solid monolith, in significant con-
All transparent nanopapers were prepared from cellu- trast to the bluish translucent silica aerogel. Therefore, it has
lose nanofibrils, which requires both energy- and chemical- attracted many interests in deriving transparent or translucent
intensive processes. Aiming at more economically favorable aerogel from nanocellulose.[52,61] Transparent cellulose nanofi-
process, researchers have been searching for much greener brils’ aerogel with 80–90% transmittance in the visible light
approaches to transforming the optically opaque cellulose regions was prepared using ordered nematic liquid crystalline
papers into transparent ones. It has been reported that by phase in cellulose nanofibril suspension (Figure 3i).[52] This
nanowelding of cellulose microfibers with 1-butyl-3-methyl- ordered liquid crystalline phase can be fixed by dilute acid
imidazolium chloride, transparent nanopaper with both high by reducing the electrostatic interactions among the surface
transparency (>90%) and haze (>90%) can be fabricated.[33,57] carboxylate groups, forming a free-standing hydrogel with
The mechanism for this direct nanopaper transformation has ordered nematic structure, which remained in aerogel after
been proposed to involve the dissolution of the surface chains supercritical drying. The aerogel then showed interesting
on cellulose microfibers by ionic liquid, which can allow them characteristics that are not commonly found within one
to entangle and weld with adjacent microfibers during hot material, including high transparency, excellent compression
pressing, to get rid of the air previously occupying the space toughness, and good heat insulation. Comprehensive research
among the microfibers. on hydrogels and aerogels containing nanocellulose has been
Besides these cellulose nanopapers, cellulose-based trans- recently reviewed in details,[62] and therefore will not be reiter-
parent nanocomposites are another type of transparent sub- ated here.
strates that have attracted numerous research interests due to
their high transparency and nonwetting surfaces. Common
to all these nanocomposites, the underlying mechanism is to 2.2. Multifunctional Mesostructures by Top-Down
infiltrate a cellulose substrate with polymer resins of matching Fabrication of Bulk Wood
refractive index, to get rid of the light scattering at the cellu-
lose–air interfaces. Starting with a translucent sheet made Although bottom-up assembly of hierarchical mesostructures
from mechanically ground cellulose nanofibers, transparent from nanocellulose building blocks has witnessed significant
nanocomposites have been made by different approaches progress over recent decades, this process requires complicated
including heat lamination between polycarbonate films, fabrication procedures with extensive chemical and energy
deposition of acrylic resin, and ink-jet printing with phenol– input from nanocellulose isolation to materials’ assembly. In
formaldehyde resin.[58] Most recently, a potentially scalable pro- contrast, wood has a natural hierarchical structure that encom-
cess in making transparent nanocomposite has been achieved passes nanoscale, microscale, and macroscale features. The
by impregnating epoxy resin on regular roll paper, showing macroscale tree trunk is comprised of vertically aligned micro-
both high optical transmittance (>85%) and high transmission channels that are responsible for water and ion transport to
haze (>90%).[59] support photosynthesis (Figure 4a).
Figure 4. Hierarchical structure of tree wood. a) Schematics showing the vascular structures of wood blocks from trees and the hierarchical structure
after delignification. Reproduced with permission.[65] Copyright 2016, Elsevier. b) SEM images of basswood after delignification, showing vertically
aligned vessels and fiber tracheid structures, which are well maintained. c) High-magnification SEM image of the cell walls, showing the presence
of pits and an unaltered cell wall structure; the inset is the photograph of white wood after delignification. d) High-magnification SEM image of the
aligned cellulose microfibrils on the cell walls in panel (c), showing the microfibrils are well aligned with numerous mesopores between the fibrils.
b–d) Reproduced with permission.[66] Copyright 2016, WILEY-VCH.
The cell wall structure of wood cells (being tracheids for soft- However, interests in designing wood-based materials with
wood or vessels and libriform fibers for hardwood) is composed advanced functionalities that have not been observed in tradi-
of lignin, hemicelluloses, and cellulose. In the cell walls of tional wood have been revived recently. Based on the treatment
wood, the secondary wall S2 layer accounts for the largest frac- and functionality, the as-fabricated wood-based advanced mate-
tion, with the cellulose microfibrils winding helically around rials include (1) transparent wood fabricated by removing the
the cell walls at certain angles relative to the long axis of cell.[9] colored lignin and filling with refractive index matching poly
Lignification of wood cell walls occurs at the final stage of xylem mers (Figure 5a,b); (2) functional transparent wood that con-
cell formation, starting from the middle lamella and S1 regions, tains functional nanoparticles (NPs) within polymer matrices
and gradually penetrating through the secondary wall toward (Figure 5c–e); (3) plasmonic wood with loaded inorganic
the lumen.[63] Lignin, as the second most abundant polymer nanoparticles for low torturous catalytic devices (Figure 5f–h);
on earth, is an amorphous branched polymer consisting of and (4) wood-based 3D, anisotropic carbon mesostructure by
crosslinked phenylpropane units. The chromophores in lignin, high-temperature carbonizing wood blocks to produce highly
such as the carbon–carbon double bonds conjugated with the conductive carbon monoliths with low tortuosity (Figure 5i–l).
aromatic rings, along with other aromatic extractives, con- Many more types of functional woods using the top-down
tribute to the dark color of wood.[64] Delignification of bulk approach are envisioned to be developed in the future.
wood by oxidative reactions or base treatment removes these
colored compounds, leaving white blocks that are essentially
aligned cellulose microfibrils (Figure 4b–d). As the middle 2.2.1. Transparent Wood
lamella is primarily composed of lignin, delignification leads to
the separation of wood cells without disintegration of the bulk Wood presents numerous structural and ecological advantages
structure. The wood cells are not altered at the microscale after but falls short in meeting the requirements for applications that
delignification, showing the same microchannel structures require optical transparency. When made transparent, wood
(Figure 4c). However, well-aligned cellulose microfibrils can can be applied in much broader areas such as windows, solar
be clearly discerned from the high-magnification SEM image, cells, and optoelectronics, to replace the traditional glass and
showing numerous mesopores between the cellulose microfi- plastics. The optical opacity of wood is ascribed to the porous
brils were created after removal of the lignin and hemicellulose cell structures that scatter lights at the air/cell wall interfaces,
previously residing among the microfibrils (Figure 4d). as well as the light-absorbing characteristics of the chromo-
Taking advantage of the hierarchical structure that naturally spheres in lignin and other extractives. Therefore, to trans-
occurred in wood, several approaches have been applied to fabri- form the opaque wood into transparent one, strategies have
cate advanced functional materials. For example, in situ polym- been proposed decades ago that include (1) chemical bleaching
erization in wood cell walls has received continued researches to remove the colored components, such as chlorophyll, tan-
to improve the existing physical properties of wood.[67] nins, and other polyphenols; (2) filling the pores with a matrix
Figure 5. a) Schematic to show the fabrication of transparent wood; b) SEM image of polymer filled transparent wood composites. The inset is photo
graph of the transparent wood. a,b) Reproduced with permission.[66] Copyright 2016, WILEY-VCH. c) Schematic and photograph of Si quantum dot
(QD) luminescent transparent wood. d) Photograph of Si QD transparent wood under 405 nm laser pumping, showing the diffused luminescence
distributed over the whole piece. c,d) Reproduced with permission.[68] Copyright 2016, WILEY-VCH. e) Transmission spectrum of transparent wood with
(red curve) and without (blue curve) rhodamine 6G (Rh6G) dye. The inset is the photograph of transparent wood embedded dye molecules. Reproduced
with permission.[69] Copyright 2017, WILEY-VCH. f) Schematic to show the in situ formation of Pd nanoparticles by hydrothermal reduction with lignin
as reducing agent. g) Photograph of the Pd NPs/wood membrane, showing Pd NPs are evenly distributed throughout the entire wood membrane.
h) TEM image of Pd NPs within the wood membrane; the inset shows the size distribution of Pd NPs. f–h) Reproduced with permission.[70] Copyright 2017,
American Chemical Society. i) Photograph of the 3D Ni/Wood carbon. The inset shows the original wood monolith. Reproduced with permission.[71]
Copyright 2016, WILEY-VCH. j) Schematic of carbon wood with low tortuosity. Reproduced with permission.[72] Copyright 2017, National Academy of
Science. k) SEM image of wood carbon showing preserved vertically aligned channel structure. l) Cross-sectional SEM image of wood carbon showing
porous structure. k,l) Reproduced with permission.[73] Copyright 2017, the Royal Society of Chemistry.
that has the same refractive index as wood (medium refractive revived in 2016, with significant progress being reported in
index of 1.54 for delignified wood and 1.56 for lignified wood making anisotropic transparent wood.[66,75]
tissue) to reduce the amount of reflection and refraction at Anisotropic transparent wood was fabricated by removing the
the interfaces.[74] To exactly match the refractive index of wood light-absorbing components in basswood through delignification
tissue, Fink synthesized co-polymers with both lower (such as treatment using sodium hydroxide, sodium sulfite, and hydrogen
poly(methacrylates), 1.48–1.50) and higher (such as polystyrene peroxide, followed by infiltration with refractive index matching
of 1.59 and polyvinylcarbazole of 1.68) refractive indices within epoxy resin (Figure 5a).[66] Complete polymer infiltration can be
chemically bleached wood, making transparent wood.[74] The observed from SEM images (Figure 5b), showing intimate associ-
research on transparent wood has silenced since then, and was ation between the resin and cell walls. The wood can be cut in two
Figure 6. a) Schematic of R-wood (top, radial direction) and L-wood (longitudinal direction, bottom) showing the lumina directions. b) Photographs of
transparent R-wood (top) and L-wood (bottom) of 2 mm in thickness. c) Schematic (top) and photograph (bottom) of incident light scattered by trans-
parent R-wood and L-wood. a–c) Reproduced with permission.[66] Copyright 2016, WILEY-VCH. d) Optical transmittance of transparent wood of 0.7 mm
made from balsa wood filled with PMMA. The inset shows the photograph of the transparent wood. Reproduced with permission.[75] Copyright 2016,
American Chemical Society. e) Photograph and SEM images of delignified white wood before pressing, showing that all the lumina structures were
preserved after delignification. f) Photograph and SEM images of transparent film pressed from the delignified white wood, showing high density and
anisotropic properties. e,f) Reproduced with permission.[79] Copyright 2017, WILEY-VCH.
directions, radially (R-wood) with the lumina channels perpen- R-wood and anisotropic scattering through transparent L-wood.
dicular to the plane direction or longitudinally (L-wood) with the Similarly, in situ polymerization of methyl methacrylate in
lumina channels parallel to the plane direction (Figure 6a), both chemically bleached balsa wood also produced transparent wood
showing clear transparency for a 3 mm thick sample (Figure 6b). with 90% light transmittance at 0.7 mm thickness, and gradu-
The transparent R-wood demonstrates up to 90% light transmit- ally decreased to 40% when the thickness increased to 3.7 mm
tance, slightly higher than the 80% light transmittance for trans- (Figure 6d).[75] This transparent wood demonstrates anisotropic
parent L-wood, possibly due to the better resin filling owing to light scattering into parallelogram due to the aligned cellulose
the vertical channel directions. The anisotropic behavior of the fibrils. In both cases, not only the transparency is significantly
transparent wood was demonstrated by the light scattering in increased by polymer infiltration, both strength and toughness
Figure 6c, showing isotropic light scattering through transparent can also be improved compared to the original wood.
With the success in fabrication of transparent wood, research and construction materials. To further expand its applica-
in fabricating more functional transparent wood has boomed, tions, complexation with plasmonic metallic nanoparticles
introducing novel properties that include tunable optical, was proposed, to offer novel functionalities that traditional
thermal, and magnetic performance. Luminescent transparent wood structures do not possess. Recently, Hu and co-workers
wood with improved diffused luminescence has been prepared successfully fabricated plasmonic wood by in situ reduction
by incorporating Si and CdSe/ZnS core/shell quantum dots, of palladium nanoparticles (Pd NPs) within wood meso-
with the luminescence diffusivity tunable by the light scattering structures using lignin as a reducing agent, representing
of transparent wood (Figure 5c,d).[68] With embedded fluorescent a green synthetic method.[70] The reduced Pd NPs can be
dye rhodamine 6G in transparent wood made from bleached capped and bound on the hydroxyls of cellulose and hemicel-
balsa wood and poly(methyl methacrylate) (PMMA), lasing effect lulose, forming a stable wood/Pd NPs’ membrane for water
with broadened laser emission spectral lines can be obtained treatment (Figure 5f). After reduction, the wood turned into
from the transparent wood employing aligned cellulose fibers black throughout the whole thickness due to the strong light
as optical resonators (Figure 5d).[69] Other than the photonic absorption by the plasmonic effects of Pd NPs anchored on
effects, magnetic transparent woods have also been reported by the surface of wood cell channels (Figure 5g). The average
incorporating ferromagnetic nanoparticles.[76] Combined with size of the Pd NPs is around 5 nm (Figure 5h), showing good
the luminescent properties, these multifunctional transparent crystallinity. The uniformly distributed Pd NPs in the wood
woods are projected to have applications in green light-emitting lumina channels served as active catalytic sites for chem-
diode (LED) lighting devices, luminescent magnetic switches, ical reduction of organic dyes, which, combined with the
and anticounterfeiting facilities. Thermal energy management wood microstructures, offer crucial characteristics for high-
in transparent wood has been achieved by adding near-infrared throughput water treatment. This application will be detailed
(NIR) radiation absorbing CsxWO3 nanoparticles in prepolymer- in the following section of sustainable application for waste-
ized methyl methacrylate resin, showing a high transparency of water treatment.
86% at 550 nm for visible light transmittance, a high haze of
over 90% from 400 to 800 nm for light diffusion, and high NIR
absorption from 780 to 2500 nm for heat shielding.[77] When 2.2.3. Wood-Based 3D, Anisotropic Carbon Mesostructure
designing wood-based sustainable materials, minimizing the
potential negative effects to biological and environmental sys- Carbonization of wood block generates monolithic wood carbon
tems should be highly prioritized. For example, CdSe has cyto- that retains vascular structures originated from the wood
toxicity and is a known carcinogen due to the release of toxic microstructures, therefore, has traditionally found applications
heavy metal ions,[78] and its incorporation should be weighed in carbon/polymer, carbon/carbon, and carbon/ceramic com-
carefully to avoid biological and environmental hazards. posites.[81,82] Due to the aligned channel structure, wood carbon
Besides transparent wood, transparent paper has also been has many advantages compared to other carbon foams derived
directly fabricated by densifying delignified wood to remove the from synthetic polymer precursors, such as anisotropic fluid
air/cellulose interfaces, which, possibly, is much more effective permeability with high liquid flux rate at the axial direction,
and scalable as compared to the transparent paper made from much higher stiffness of ≈10 GPa in the aligned axial direc-
CNF. After delignification, the colored wood turns white due to tion, one order of magnitude higher than the isotropic carbon
the removal of color-absorbing chromophores while the aligned foam.[81]
channel structures are retained, as the cellulose microfibril With increasing concerns on sustainability, interest in wood
skeleton is well preserved (Figure 6e).[79] After compressing, the carbon monoliths has revived to address more emerging appli-
white wood turns into a transparent film with five times reduc- cations, such as in sustainable and renewable energy, high
tion in thickness, having a dense cross section with very low porosity for active materials loading, and accommodating
roughness (Figure 6f). Chemical treatment and densification lithium expansion/contraction during stripping/plating in bat-
do not alter the cellulose crystalline structure or the microfibril teries (Figure 5i,j). Carbonization of basswood at 1000 °C in Ar
alignment, resulting in anisotropically aligned all-cellulose produced a wood carbon monolith with preserved lumina chan-
I films with a high tensile strength of 350 MPa and a toughness nels ranging from 5 to 60 µm wide (Figure 5k,l).[72] This wood
of 7.38 MJ m−3, both are three times higher than the isotropic carbon shows distinct characteristics of high porosity (73%),
transparent nanopaper with randomly oriented cellulose low tortuosity, and disordered amorphous feature (I(D)/I(G) of
nanofibrils. Besides, as the lumina channels that scatter inci- 1.26 from Raman spectra), and has been demonstrated to be
dent light were removed by compressing, the directly fabricated used as lithium metal host in lithium-ion battery (LIB)[72] and
transparent nanopaper showed over 90% light transmittance as anode/cathode materials for supercapacitors.[73] Functional
well as high haze, which has been demonstrated in applications wood carbon has also been prepared by impregnating wood
for light management in solar cells with a significant efficiency with metal precursors, which, upon high-temperature pyrolysis,
enhancement of 14%.[80] can be reduced as metallic nanoparticle catalysts loaded on the
wood carbon.[71] The Ni-nanoparticle-decorated wood carbon
has been demonstrated as a 3D flow-through wood-carbon-sup-
2.2.2. Plasmonic Wood ported catalysts, to be used in steam reforming of biomass tars.
Detailed application of wood carbon in energy storage devices
Due to the limited functionalities, wood-based materials have will appear in the following account on sustainable applications
been primarily limited in traditional applications as building for energy storage devices.
3. Sustainable Application: Transparent Paper Improved performance of transparent paper has been dem-
to Replace Plastic onstrated over the years including better optical properties,
mechanical properties, surface morphologies, and modified
Plastic exhibits many advantageous qualities such as flexibility, functionalities. Different fabrication techniques have been
durability, and cost–effectiveness. Consequently, plastics have developed including use of dissolved cellulose, nanofibril-
been ubiquitously used in our daily lives in construction, deco- lated cellulose (NFC), and even direct pressing of delignified
ration, packaging, electronic devices, encapsulations, and many wood.[39,79,80,87] Owing to the hierarchical structure comprising
other areas. Substrates play a critical role in flexible electronics. well-oriented microfibrils and elementary fibrils in cellulose,
Plastic is often used as a substrate or packaging for electronic the optical and mechanical properties of cellulose paper can
devices. However, plastic is not environmentally friendly, and thus be tuned. Unlike plastics, the optical transmittance and
is known to be resistant to biodegradation (Figure 7a,b). Plastic scattering of transparent paper can be modulated for varied
takes up significant space in landfills, ≈8 million metric tons of application scenarios.[51,56,88] The cellulose paper composed
plastic waste end up in oceans every year, with the total amount of nanosized fibers exhibits smoothness comparable to that
increasing by an order of magnitude by 2025.[83] Another of plastic. Meanwhile, since the fiber size is smaller than the
alarming fact is that the indestructible plastic waste can also wavelength of visible range photons, light can be directly trans-
release toxic substances into seawater, greatly endangering the mitted with minimal scattering effects.[51,86] On the other hand,
living conditions of humans and other species.[83,84] Moreover, the cellulose paper composed of microsized cellulose can sub-
most plastics are synthesized from petroleum, which has lim- stantially scatter light with a high haze, to increase forward
ited reserves. In addition, burning plastics can be especially light-scattering and eliminating glare effect.[89]
problematic (Figure 7c), with polyvinyl chloride, in particular, Optically transparent paper with a super-smooth surface can
contributing to high emissions of dioxin, which can cause rival plastics and propel flexible, even foldable, green electronics.
acute respiratory and other health problems.[85] Therefore, a There have been several works reporting super-clear trans-
rising presence of plastic waste has raised substantial concerns, parent paper.[33,62] Hu and co-workers fabricated mesoporous
and driven the continuous search for sustainable materials to cellulose structures with tailored optical, mechanical, thermal,
replace plastic. Transparent paper derived completely from trees and electrical properties from pure wood cellulose nanofibers
is a promising alternative. Trees are of abundant source and (Figure 8a).[33] A super-clear transparent paper (Figure 8b) has
can promote carbon sink instead of carbon emission. Trans- been demonstrated with optical transmittance comparable to
parent paper can be completely biodegradable (Figure 7d), as that of plastics (up to 92% as shown in Figure 8c). A haze as
cellulose can be easily broken down by natural means, typically low as <1% was obtained (Figure 8d), which was even lower
in the periods of less than several months.[86] than that of poly(ethylene terephthalate) (PET). The nanoscale
Figure 7. Comparison between plastic and transparent paper. Plastics are synthesized from petroleum, which is a limited resource, while cellulose-
derived products can exhibit the same desirable properties while supporting a healthy and sustainable environment. a) Plastic waste accumulates and
cannot degrade. b) Plastic pollution on the seabed. a,b) Reproduced with permission.[84] c) Toxic aerosols generated from plastic burning. Reproduced
with permission.[85] Copyright 2015, Elsevier. d) As a promising alternative to plastic, transparent paper is composed of sustainable and biodegrad-
able cellulose from trees. In addition, added functionality has been realized with transparent paper such as tunable light management capabilities.
Reproduced with permission.[86] Copyright 2015, Macmillan Publishers Limited.
Figure 8. Super clear transparent paper to replace plastic. a) Cellulose nanofibers derived from wood cellulose. b) Photograph of super-clear paper
with a dimension of 20 cm × 20 cm. c) Total forward light transmittance and d) transmittance haze for clear paper, flexible glass, and PET plastic.
e) Laser cutting process of graphene on super-clear paper. f) The linearity test of patterned super-clear paper. Reproduced with permission.[33]
Copyright 2015, American Chemical Society.
morphology of cellulose fibers was smooth and optically trans- It is clear that in the electronic substrate area normally domi-
parent, which can minimize the scattering effects of incoming nated by transparent plastics, super-clear transparent paper can
light. The extremely low haze of transparent paper makes it directly replace plastic with its high transparency, low haze, and
promising for a wide range of optoelectronic applications that nanoscale surface roughness. In addition, super-clear paper
require high clarity such as high-quality flexible displays and also exhibits excellent biodegradability that is more environ-
clear coatings for touch screens. As a demonstration, the authors mentally responsive.
used the super-clear paper as a multipoint capacitive-based More recent works show that the transparent cellulose
touch screen with a deposited graphene layer as conducting paper with high haze can be used as a light management
electrode patterned by a laser cutting method (Figure 8e). The layer for solar cells and LEDs with increased light-coupling
patterned clear paper was tested on the linearity performance efficiency. The large light scattering effect cannot be real-
to demonstrate the accuracy of touch sensing. When the user’s ized in plastic without sacrificing transmission. In sharp con-
finger is moved along a straight line, the device incorporated trast, transparent paper with both high transparency and high
with a transparent cellulose paper touch screen responds to the haze could be achieved simultaneously by adjusting the fiber
exact locations, showing a linear line on the monitor (Figure 8f). dimensions. When used as light management layers for opto-
The authors also conducted a commercial-grade durability test electronic devices, both high transparency and high haze are
by bending the paper device repeatedly 10 000 times. On top necessary to reduce shadowing effect while increasing index
of its excellent performance demonstration, the screen is also matching and photon travelling path in active layer of optoelec-
completely biodegradable, making it attractive for the appli- tronic devices. A novel structure with pure wood cellulose was
cations of consumer electronics with increasingly shortened reported, achieving both super high optical transmittance and
lifespans. haze (Figure 9a),[51] where the paper was used for light manage-
Due to its unique properties such as foldability and hydro- ment coating of solar cells. An improved solar energy conver-
philicity, the cellulose paper can also be used as substrate for sion efficiency of organic solar cell was observed (Figure 9b).
foldable devices and microfluidic devices. A foldable nanopaper When a green laser beam was used to illuminate the hazy
antenna was demonstrated by Nogi et al.[90] Transistors,[91] LED paper, a greatly scattered transmittance pattern was observed
displays,[92] and conductive transparent paper[93] were dem- (Figure 9c). Similarly, the high-transmittance and high-haze
onstrated with cellulose papers. Fluidic devices such as ionic paper can also be applied in the LEDs (Figure 9d). The index
diode[94] and microfluidic applications[95] have also gained matching provided by the paper coating layer, and the greatly
increasing attention. With an MoS2 transistor patterned on increased photon scattering facilitated enhanced light coupling
super-clear cellulose nanocrystal paper, Tao et al. also demon- of the optoelectronic devices (Figure 9e). A higher conversion
strated that the nanoscale roughness of the fabricated paper efficiency was thus observed in both solar cells and LEDs after
surface is ideal for microsized or even nanosized devices.[62] All transparent paper coating. A roll of high-transparency and
of these demonstrate the wide applicability of cellulose paper in high-haze paper was demonstrated with a large-scale and
electronic and fluidic devices. industry-compatible roll-to-roll process (Figure 9f).[56] The
Figure 9. Light management of high haze transparent paper. a) Photograph of a transparent paper with high haze. b) An organic solar cell exhib-
iting improved efficiency after coating with high-haze transparent paper. c) When illuminated with a green laser beam, the transmitted pattern was
largely diffused. a–c) Reproduced with permission.[51] Copyright 2013, American Chemical Society. d) LED coated with high-haze transparent paper.
e) The effect of paper coating on the LED. Increased light scattering and index matching between air and device both contribute to a high LED illumination
efficiency. f) Large-scale process of transparent hazy paper. d–f) Reproduced with permission.[56] Copyright 2016, the Royal Society of Chemistry.
paper was a cellulose paper infiltrated with epoxy resin that (Figure 10c). The fungus fully covers the transparent paper film
realized the optical management capability of high-haze cel- after 60 d. Once degraded, the left-over circuit can be further
lulose paper. The epoxy resin was used to create a refrac- decomposed and recycled. The patterned devices are also flex-
tive-index-matching matrix with enhanced transparency, and ible, which can lead to more possibilities in the applications of
the microsized cellulose fibers can scatter light to achieve high wearable electronics.
optical haze. Besides paper-based transistors, biodegradable devices
Most consumer electronics, such as smartphones, tablets, including organic LEDs and organic solar cells have also been
and watches, are based on integrated circuits. Most of the demonstrated using transparent paper, showing improved
chips that these devices use are made from silicon or III–V performance over those on plastic counterparts due to their
semiconductor materials for computing and optical sensing. unique light management capabilities.[33,41,91,96] Kippelen and
However, the amount of waste from electronic products has co-workers reported an easily recyclable organic solar cell
rapidly grown over the past years, requiring more landfill space patterned paper with an efficiency of 2.7% (Figure 11a),[97]
to accommodate disposal. In addition, the disposal of the elec- which is comparable to the efficiency of a solar cell patterned
tronic devices can release toxic substances into the landfill such on plastic film. The solar cell film exhibits an open-circuit
as heavy metals and toxic elements, which presents concerns voltage of 0.65 V and a short-circuit current density of
about jeopardizing the safety of drinking water. Thus, the utili- 7.5 mA cm−2 while a fill factor of 0.54 (Figure 11b). The trans-
zation of a biodegradable and environmentally friendly alterna- parent paper was patterned with silver on both sides as elec-
tive as the substrate of electronic devices and electronic pack- trodes (Figure 11c), which can be facilely burned in less than
aging is highly desirable. 2 s with minimal smoke, and the entire device quickly became
Ma and co-workers presented the possibility of integrating a residue of ashes (Figure 11d), without releasing toxins as is
functional circuits with transparent paper.[86] The main compo- the case for plastic.
nent of the transparent paper is completely derived from trees, In summary, rapid progress and growing interest in utilizing
and therefore can be completely degraded and is sustainably cellulose paper for a wide range of applications in replacement
compatible with land disposal (Figure 10a). The transmittance of plastics have been witnessed in recent years. Moreover, addi-
of the demonstrated paper is over 80%, making it ideal for tional functionalities of cellulose paper have been reported such
certain optical applications. Figure 10b shows the microwave- as tunable optical and mechanical properties, enabling cellulose
active GaAs electronic device on transparent cellulose paper. paper with more advanced applications that are not possible for
The patterned circuit is an array of heterojunction bipolar tran- plastics. Improved understanding of fundamental properties
sistors. The transparent-paper-based devices greatly reduce and further development of processing techniques of trans-
the use of expensive and hazardous semiconductor materials. parent paper enables demonstrations of more and more proof-
The as-made devices can be degraded completely by fungi of-concept devices with excellent mechanical flexibility, and
Figure 10. Biodegradability of paper-based functional electrical circuit. a) The lifecycle of transparent paper electrical circuit. b) An array of GaAs
devices that patterned on the transparent paper. c) The process of fungal degradation on paper-based integrated chip. Reproduced with permission.[86]
Copyright 2015, Macmillan Publishers Limited.
even bendability. However, challenges remain to fully replace can reduce carbon footprint while yielding financial savings.
plastic with cellulose paper in daily applications including the Effective and consistent sunlight harvesting can substantially
nanofabrication complexities, energy consumption in fabrica- reduce electrical usage while promoting natural and comfort-
tion, substrate property improvements such as durability, per- able indoor lighting. In addition, the indoor environment is of
formance stability, water resistivity, and reliability of large-scale great significance to occupants’ health, working efficiency, and
production. For example, cellulose paper exhibits a low water thermal comfort. In recent years, the topic has attracted sub-
resistivity compared with plastic film due to the inherent hydro- stantial interest in the energy-saving building sectors.
philic functional groups, requiring the development of surface Glass is the most commonly used material for buildings
encapsulation techniques to improve water stability.[56] In order and solar panels. However, glass is of very low energy effi-
to further increase cost–effectiveness of large-scale-production ciency mainly due to two reasons: (1) glass often creates shad-
cellulose paper, the complexities and the energy consumption owing effects and uncomfortable glare, which would require
associated with fabrication need to be reduced. Following the daytime lighting to meet the occupants’ needs; (2) one third
challenges is a wave of new research on improving the cost– of the energy used to heat or cool the building is lost through
effectiveness of transparent cellulose paper by enhancing mor- inefficient glass windows due to its intrinsic high thermal
phology stability under various conditions and developing new, conductivity.[98] Glass also presents significant safety concerns
reduced cost fabrication methods. Cellulose-based transparent when used in residential and commercial structures. When
paper also exhibits properties that cannot be realized by tradi- it undergoes a sudden impact such as flying debris, an earth-
tional plastic such as integration of microfluidic functionality, quake, or even sudden movement of the occupants, glass can
foldability, and printability. The future development of trans- break and spray shattered pieces in all directions. Sometimes
parent paper will not only help replace conventional usage of glass can have sudden and spontaneous failure caused by edge
plastic but also enable applications in a wide range of new areas. or surface damage that propagates through creep loads.
Transparent wood has the potential to replace glass with the
following advantages:
4. Sustainable Application: Transparent Wood to
(1) Antishatter: While glass shatters immediately into pointed
Replace Glass
shards upon mechanical shock, transparent wood stays
As promoted by the U.S. Department of Energy, energy intact, which is highly desirable as a safe, hassle-free, and
consumption of buildings is required to be reduced 20% antishatter transparent building material.
by 2020, and 50% as the long-term goal.[98] Light management (2) Environmentally friendly: According to the report from the
in green building is of critical importance. Lighting and air-con- nonprofit environmental organization Clean Air Council in
ditioning usage accounts for over 70% of all the energy used in 2008, only 23.1% of discarded glass was recycled.[99] Now,
commercial and residential buildings. Better thermal insulation with landfills across the planet, glass is rapidly becoming a
in buildings by adoption of substantial construction materials major ingredient in pockets of Earth’s crust, and it will not
Figure 11. Bio-degradable paper-based solar cells. a) Photograph of a recyclable and transparent paper organic solar cell. b) The current–voltage char-
acterization of the fabricated solar cell—black curve: dark characterization of solar cell; red curve: solar cell performance under 1 sun illumination. c)
Silver contact deposited on both sides of solar cell. d) The fabricated solar cell burned immediately and left minimal residue. Reproduced under the
terms of the CC-BY 4.0 license.[97] Copyright 2013, The Authors, published by Macmillan Publisher Limited.
decompose anytime soon. On the other hand, transparent direction regardless of the position of the light source. When
wood is biodegradable, which will substantially reduce the used for building materials, the transparent wood can help
presence of discarded windows and glassware in landfills. to reduce the daytime lighting energy use while also creating
(3) Energy efficiency: Transparent wood as a building material a comfortable and consistent indoor lighting environment.
can efficiently guide sunlight to provide consistent and uni- Meanwhile, transparent wood provides a lower thermal con-
form indoor lighting for buildings without a glare effect. ductivity compared to glass, indicating a better thermal protec-
The transparent wood composite also has much better ther- tion of the house. Owing to the naturally formed alignment in
mal insulation than glass, which will help improve thermal wood, the thermal transport along and across the wood channel
energy efficiency in houses and automobiles. In compari- direction is highly anisotropic. In wood cross-plane direction,
son with the limited light management capability of glass the thermal conductivity is only 0.12 W mK−1. Given the filling
(Figure 12a), the advanced light guiding effect of transparent material epoxy exhibits an intrinsically high thermal conduc-
wood is illustrated in Figure 12b. tivity of 0.60 W mK−1, the low thermal conductivity obtained
in transparent wood suggested the effectiveness of wood fiber
Sunlight is the most natural light that can promote human boundaries in lowering heat transport. Other properties have
health and at the same time reduce artificial lighting use. As also been discussed, such as the improved mechanical tough-
a demonstration, transparent wood can be used as an energy ness over glass. The authors also show after 3 d immersion in
efficient building material (Figure 13a), facilitating effective water, no visible morphology change was observed in the trans-
daylight harvesting and thermal insulation to reduce electricity parent wood, indicating an enhanced stability of performance.
usage and weatherization cost, to replace glass that only has The simple, scalable fabrication of transparent wood with reli-
limited light management capability and poor thermal insula- able performance shows great promise of transparent wood as
tion.[100] The naturally formed channels inside wood that once a future building material, especially as a replacement of glass
responsible for water and ion transport can now guide sunlight toward energy-efficient buildings.
into the buildings (Figure 13b), resulting in a uniform and There has been great progress in solar cell efficiency by the
consistent daylight distribution over the day without glare. A recognition of the need to increase photon travelling paths by
transparent wood roof was installed on a house model to com- surface texturing.[101] However, the fabrication for surface pat-
pare with a glass roof house. The wood-roofed house could terning is usually expensive and complicated, thus greatly lim-
achieve more uniform interior illumination due to the light iting its scalability and cost control. Recently, Hu and co-workers
guiding and scattering effect of transparent wood (Figure 13c). demonstrated the unique optical properties of transparent
The light guiding effect is illustrated in Figure 13d. A green wood showing an extremely high haze of 80% (Figure 14a).[65]
laser (532 nm) beam was used to illuminate the transparent Meanwhile, the transparent wood also exhibited a broadband
wood sample (1.4 cm thick) at different angles. The light pas- transmittance as high as 92%, which is comparable to that of
sage within the wood sample occurred along the wood channel glass (Figure 14b). The substantially enhanced light scattering
Figure 12. Comparison between glass and transparent wood. a) Glass is not energy efficient and exhibits safety and environmental concerns. b) On the
contrary, transparent wood can provide reduced daytime lighting usage and weatherization cost, and it is more environmentally friendly. Reproduced
with permission.[100] Copyright 2016, WILEY-VCH.
effect in transparent wood can thus potentially be used as light GaAs has been studied as one of the most promising
management coatings for optoelectronics devices such as LEDs high-efficiency thin-film materials.[102] For such solar cells
and solar cells. with a high absorption coefficient, the active region for light
Figure 13. Transparent wood for energy efficient buildings. a) Schematics of using transparent wood as energy-efficient building materials.
b) SEM image of aligned lumens in wood. After wood is made transparent, light can be guided along the lumen direction. c) A glass and a transparent
wood were used as the roof of a house model. Light intensity at different spots inside the house model was measured. The transparent wood roof
yields a more uniform light distribution inside. d) A collimated visible laser beam irradiates the transparent wood. The light passes along the lumen
direction independent of the incident angle. Reproduced with permission.[100] Copyright 2016, WILEY-VCH.
Figure 14. Transparent wood for solar cells. a,b) Transparent wood exhibits a high haze of ≈80% (a) and a high transmittance of ≈90% (b). c) Schematics
of the transparent wood coating on solar cells. Owing to the high diffusive transmittance of transparent wood, it can function as a light management
layer for solar cells. d) An 18% efficiency enhancement was observed after coating. Reproduced with permission.[65] Copyright 2016, Elsevier.
absorption is generally only in the order of several micrometers. The wood encapsulation to the cell can also assist the long-term
In fact, only the top 3 µm thick GaAs layer is responsible for surface protection.
the light–electricity conversion. The hundreds of micrometers Besides, owing to its unique light and thermal management
of GaAs substrate are very expensive and will greatly raise the capabilities along with high mechanical toughness and sustain-
overall dollars-per-watt value of the cell. In order to reduce the ability, transparent wood has also been demonstrated for many
material cost, the active layer will generally be transferred to a other applications in optoelectronic devices, light-harvesting
much less expensive substrate followed by an epitaxial lift-off materials, and transparent matrices for incorporation into infil-
process.[103] In this way, the GaAs substrate can be reused for trated functional materials,[68,76,77] to potentially replace glass.
the growth process multiple times. The demonstrated trans- Although there are other low-cost alternatives to transparent
parent wood is a superb candidate as the transfer substrate. It paper or wood, for example, silicon-based materials,[104] they all
is flexible and robust with controllable thickness. It can support present some disadvantages over the transparent paper or wood
the thin-film materials such as GaAs for flexible application. It in terms of both mechanical and optical properties. First, sil-
is highly transparent with an extremely high haze. When illu- icon is typically fragile with low mechanical toughness, whereas
minated from the back side (substrate side), the wood can func- wood-based materials such as transparent wood or cellulose
tion as both a surface scattering layer and an index matching paper are more flexible and tough. Second, silicon exhibits an
layer, substantially increasing the photon travelling path and, at intrinsically high absorption coefficient over visible light, which
the same time, reducing the surface reflection loss (Figure 14c). renders it unsuitable for applications that require high trans-
Experimentally, an enhancement of 16% was observed in short- parency. On the contrary, cellulose-based transparent wood
circuit density under 1 sun illumination and a corresponding and paper demonstrate negligible absorption within the vis-
18% overall conversion efficiency boost (Figure 14d). Consid- ible wavelength range after removing the light-absorbing lignin
ering the shadowing effects after applying transparent wood on through delignification and infiltration of index-matching
the cell (the transparency of the wood is less than 100%), the polymers to reduce scattering at the air–cellulose interfaces.[66]
enhancement percentage on the light-scattering effect should Although other Si-based dielectric materials such as Si3N4 and
be even larger. A slight enhancement of fill factor from 75.06% SiO2 can effectively transmit light within visible range, these
to 76.04% has also been observed. The fill factor serves as a materials often exhibit wavelength-dependent absorption coef-
good indicator of the dark saturation current density change. ficients.[105] In contrast, cellulose-based transparent wood and
The exposure of GaAs surface to air can slowly degrade the cell paper exhibit a nearly constant transmittance over the entire
by creating surface dangling bonds and facilitating nonradia- visible range (400–700 nm). This broadband transmittance
tive recombination of the light-generated electron–hole pairs. effect is highly desirable for applications that require more
vivid image transmission. Therefore, it is not ideal for silicon 5. Sustainable Application: Super Strong
to replace plastics and glass in applications that requires high Materials for Structural Applications
transparency.
In conclusion, transparent wood exhibits unique light and Although wood has been used as structural building material
thermal management capabilities such as light-guiding effect, for thousands of years, its dominant role in construction has
large forward scattering, and thermal resistance from the been largely overtaken by man-made structural materials, such
numerous heat transfer interfaces. Transparent wood is also as steel and cement, due to the lack of sufficient mechanical
derived from biodegradable and sustainable sources. Unlike performance. However, from the sustainability point of view,
glass, transparent wood can withstand high impact energy using wood-based materials has much lower impact to the envi-
and prevent sudden shattering, which is much safer to use in ronment considering the minimal industrial processing, as well
daily lives. Therefore, it can be used toward a wide range of as neutral or even negative carbon dioxide emission if the wood
applications including energy-efficient building material, light- is not incinerated at the end of its life.[106] Compared to wood,
harvesting panels, functional matrix, and light management steel production contributes much more energy consumption
coatings. However, in the current stage, main technological and CO2 emission (25.5% vs 1.5% energy consumption and
hurdles for transparent wood to replace glass are to modulate 18.7% vs 1.1% CO2 emission for steel and wood, respectively)
clarity of the material, i.e., to achieve low optical haze (1%) for (Figure 15a).[106] Besides lower energy consumption and CO2
applications that require minimized distortion of transmitted emission, wood-based materials have numerous other advan-
optical images.[66] Another concern for realistic applications is tages that include light weight, low thermal expansion, and
the capability for large-scale production with reduced cost that high specific strength and Young’s modulus, with some of the
can compete with the production of glass. Besides, UV sta- reported values even greater than that of steel (Figure 15b). In
bility and uniformity of large-scale production also need to be fact, the highly crystalline cellulose nanofibrils show extraor-
improved for realistic applications. For example, without cor- dinary mechanical properties including 120–220 GPa Young’s
rective techniques in place, the transparent wood is known to modulus[1,30] and 1.6–3 GPa strength,[31] comparable to those
develop a yellowish color over time due to UV irradiation and of multiwalled carbon nanotube (CNT) and synthetic Kevlar
can exhibit slightly different optical and mechanical properties fibers.[1,31] Therefore, it has been proposed that nanocellulose-
when made from wood sourced from different parts of a tree. based materials could be used to replace steel for structural
Since the development of transparent wood is still at its very applications.[27] In this section, the mechanical properties of
early stage, more functionalities and applications will be devel- materials derived from cellulose nanofibrils will be the primary
oped in the future with improved process techniques and new focus for exploration of their potential to replace steel.
selections of infiltration materials. The direction of the research Recently, tremendous effort has been devoted in designing
of highly functioned transparent wood can achieve new proper- ultrastrong cellulose I macrofibers, primarily through wet-
ties and enable new applications that glass could not realize. extrusion of cellulose nanofibril aqueous suspensions into a
Figure 15. Comparison between steel and wood-based materials. a) Contribution of energy demand for the manufacture of the materials needed in
the construction of 1 m2. Reproduced with permission.[106] Copyright 2010, Elsevier. b) Specific ultimate strength versus specific Young’s modulus
of different materials. The angle represents the CNF alignment relative to the axis of the filaments. Reproduced with permission.[37] Copyright 2014,
Macmillan Publishers Limited.
coagulation bath. To achieve improved mechanical properties, strength as high as 490 MPa and Young’s modulus of 18 GPa
various techniques have been employed to align the cellulose (Figure 16c). The specific strength and modulus of the cellulose
nanofibrils along the axis of macrofibers. As CNF suspension is fibers increased with improved CNF alignment, or a decrease
pushed through a syringe needle during spinning, CNFs expe- of the angle between cellulose nanofibrils and axis of filament
rience shearing forces, which leads to their partial alignment.[34] (Figure 16d). For cellulose fibers with fully aligned cellulose
However, it has been found that pure shearing force is insuffi- nanofibrils, the specific strength and modulus are comparable
cient for complete CNF alignment, therefore leading to only a to synthetic fibers such as glass fiber and Kevlar.
moderate Young’s modulus of 22.5 GPa and a tensile strength Similar to macrofibers, cellulose nanofibrils’ film with
of 275 MPa, still one order of magnitude lower than that for cel- improved mechanical properties can also be prepared by cold
lulose nanofibrils. Increasing the spinning rate leads to higher drawing of the CNF hydrogel cake shaped by filtration.[107]
shearing force, therefore, can significantly improve the tensile The mechanical properties are significantly improved with
strength from 90 to 321 MPa and Young’s modulus from 8.4 to increased draw ratio up to 1.6, with the Young’s modulus
23.6 GPa with increased spinning rate from 0.1 to 100 m min−1, increasing from 10.3 to 33.3 GPa and the tensile strength
which is ascribed to better CNF alignment.[34] increasing from 185 to 397 MPa (Figure 17a). The enhanced
Wet stretching represents an effective way in aligning cellu- mechanical properties correspond well to increased degree of
lose nanofibrils in the axis direction. With stretching ratio up to orientation, which can reach as high as 82% and 89% in the
1.3, the Young’s modulus and tensile strength increased quad- plane and at the cross-sectional plane, respectively. The Young’s
ruply from 8.2 to 33.7 GPa and doubly from 118 to 289 MPa, modulus also increased linearly with the drawing ratio. Mon-
respectively.[36] Although the 289 MPa tensile strength is less olayer grafting of TEMPO-oxidized cellulose nanofibrils with
than the previously reported 321 MPa, the Young’s modulus 0.7 nm thick poly(ethylene glycol) can prevent CNF agglom-
increased over 10 GPa after stretching. Recently, a more com- eration, thus facilitating alignment into compartmentalized
plicated hydrodynamic alignment was adopted to align cellu- fibril bundles upon mechanical stretching.[52] Therefore, with
lose nanofibrils in the flow direction, followed by immediate increased PEG grafting density, the mechanical properties of
gel fixation by electrolyte diffusion to maintain the aligned the CNF ribbons increased from 17.2 to 32.3 GPa for Young’s
structure (Figure 16a).[37] The SEM image of the filament modulus and from 388 to 576 MPa for tensile strength at the
showed void-free and homogeneous cross section, without highest grafting density of 33% weight fraction (Figure 17b).
signs of individual nanofibers (Figure 16b). This dense and Compared to the mechanical properties of CNF-g-PEG-33
compact structure comes from the dual effects of alignment ribbon without stretching (6.4 GPa Young’s modulus and
and fixation, resulting strong and stiff filament with the tensile 220 MPa tensile strength), these values are significantly higher
Figure 16. a) Schematic to show the hydrodynamic alignment of cellulose nanofibrils followed by electrolyte diffusion to induce gelation. b) SEM image
of the cellulose nanofibrils filaments. c) Stress–strain curves of different cellulose nanofibrils filaments. d) Specific ultimate strength versus specific
Young’s modulus of different materials. The angle represents the CNF alignment relative to the axis of the filaments. Reproduced with permission.[37]
Copyright 2014, Macmillan Publishers Limited.
Figure 17. a) Tensile stress–strain curves of TEMPO-NFC nanopaper with different draw ratios (DR). Reproduced with permission.[107] Copyright
2012, American Chemical Society. b) Stress–strain curves of nonstretched (N) and stretched (S) PEG-grafted cellulose nanofibrils ribbons.
c,d) AFM height images showing the surfaces of the nonstretched (c) and stretched (d) CNF ribbons. e) X-ray diffractograms of the surface planes.
b–e) Reproduced with permission.[52] Copyright 2015, Wiley-VCH.
due to the preferential orientation of the aligned nanofibrils offering mechanical support to trees. Reconstructing cel-
(Figure 17c,d). Wide-angle X-ray diffraction further confirmed lulose nanofibrils into strong and tough materials has been
the preferential orientation by showing the equatorial arc after extensively investigated, aiming to mimic and excel the nat-
stretching (Figure 17e). Higher grafting density leads to higher ural wood. The mechanical properties of cellulose nanopaper
orientation index, suggesting that the grafted PEG facilitates the depend highly on the degree of polymerization of the cellulose
alignment of the cellulose nanofibrils by interfacial lubrication. molecules in the nanofibrils.[109] With increasing degree of
Strength and toughness have generally been regarded as polymerization from 410 to 1100, the tensile strength increased
mutually exclusive, considering the most common combina- significantly from 129 to 214 MPa, and the work of fracture
tion of “strong but brittle” and “tough but weak.”[27,108] There- (an indicator for toughness) increased five times from 3 to
fore, the quest for strong and tough engineering materials has 15.1 MJ m−3. This simultaneous enhancement in both strength
sparked great research enthusiasm, and progress has been and toughness is of great interest for this nanofibrils network
made through learning from naturally occurring materials, structure. Recently, Hu and co-workers discovered an anoma-
such as bones, nacre, and wood.[108] As the basic building blocks lous but highly desirable scaling law of the cellulose nanopaper:
of wood, cellulose nanofibrils bind with each other through the smaller, the stronger and the tougher (Figure 18a), as indi-
interfibril hydrogen bonding and van der Waals interactions, cated by the simultaneous increase in both the toughness and
Figure 18. a) An anomalous but desirable scaling law of mechanical properties requires defeating the conventional conflict between strengths and
toughness. b) Both tensile strength and toughness increase significantly as the cellulose fiber diameter decreases from micrometer to nanometer scale.
(c) Stress–strain curves of cellulose paper made of cellulose fibers of various mean diameters. d) Ultimate tensile strength scales inversely with the
square root of cellulose fiber diameter. Reproduced with permission.[27] Copyright 2015, National Academy of Science.
ultimate tensile strength with the decrease of mean cellulose and hurdles are present for the bulk materials of several inches
fiber diameter from 27 µm to 11 nm (Figure 18b).[27] The tensile in thickness to match these mechanical performance. Besides,
strength increased 40 times from 6.7 to 275.2 MPa as the fiber most of the current research on wood- or cellulose-based struc-
diameter decrease from 27 µm to 11 nm (Figure 18c), which tural materials focus on the strength and modulus values,
is inversely proportional to the square root of fiber diameters without giving strong emphasis to the mechanical toughness
(Figure 18d). Simultaneously, the toughness increased nearly improvement.[37,52] Strong and tough materials’ development
130 times from 0.13 to 11.68 MJ m−3, and the fracture tough- should call for continued investigation. Additionally, as a
ness increased more than 10 times from 143.3 to 1481.4 J m−2. structural material, wood needs additional treatment for fire-
Through a continuum fracture mechanics model, it is proposed resistant and antifungal properties, which can be potentially
that this anomalous scaling law of strength and toughness hazardous to environment. Nevertheless, more interest has
increment can be ascribed to the reduced intrinsic defect size been given to wood as a construction material for buildings,
and the formation and reformation of strong hydrogen bonding and the final success in converting to wood structures requires
among cellulose chains. continuous efforts on both regulating the building codes and
In essence, the extraordinary mechanical properties of highly developing engineering and technical skills.[111]
crystalline cellulose nanofibrils make them excellent candidates
for assembling strong and tough materials that could poten-
tially replace steel for lightweight construction materials. How- 6. Sustainable Application: Wood-Based Energy
ever, to realize this ambition, there will still be long way ahead
Storage Technologies
to further improve the mechanical performance and promote
large-scale production. First, although significant progress has Nowadays, the rapidly growing demand for energy calls for
been made in improving the mechanical properties of cellulose cleaner and more renewable energy. However, it is still chal-
nanofibril-based materials, there are still great challenges in lenging to integrate clean energy into the grid due to the
fully transferring the mechanical properties of individual cel- intermittence of renewable energy.[112] Thus, advanced energy
lulose nanofibril to the macroscopic assembled forms.[110] To conversion and storage systems with high energy density and
bridge the gaps between nanoscale and macroscale mechan- high power density are highly desired.[113] Meanwhile, with
ical properties, novel design strategies need to be developed, the increasing environmental awareness, sustainability and
to improve fibril alignment, enhance interfibril bonding, and eco-friendliness should be taken into consideration for develo
reduce intrinsic defects. Second, the superb mechanical per- ping energy conversion and storage devices.[114] Wood and its
formance of the crystalline cellulose-based structural materials derived materials have shown great promise in energy-related
is generally reported on the forms of fibers or thin films with studies due to their earth abundance, light weight, and biodeg-
very small cross-sectional areas,[52] whereas great challenges radability.[2] To date, wood-based materials are designed to act as
current collectors, separators, green binders, and unique hosts where ε, D, and DT mean the porosity, the conductivity of the
for electrode materials. In this section, we will highlight the electrolyte, and the macroscopic diffusivity, respectively.
applications of wood and its derived materials in different kinds Inspired by the inherently aligned, straight channels of
of energy conversion and storage devices toward sustainability. wood, Hu and co-workers proposed a novel electrode configu-
ration design by loading active materials into channels of car-
bonized wood (C-wood; Figure 19b), where the unique wood
6.1. 3D Carbon to Replace Metallic Current Collector architecture functions as a perfect current collector for thick
electrode design. With such a design, the carbonized wood
Currently, lithium ion batteries (LIBs are the main power source framework with aligned channels provides connected path-
for portable devices due to their high energy density.[115] To fur- ways for fast electron transport (Figure 20a).[120] Furthermore,
ther increase the energy density of LIBs), considerable studies this carbon framework possesses a high porosity of 81%, which
have been devoted to developing new electrode materials.[116] provides sufficient contact with electrolyte, low tortuosity, and
On the other hand, optimizing the battery electrode configu- spatial space for holding high mass loading of the electroactive
ration can improve the energy density of LIBs as well.[117] For electrode materials. Moreover, the wood-based current collector
example, conductive additives, binders, and current collectors is much more biodegradable and sustainable than metallic cur-
do not contribute capacity in the conventional electrode configu- rent collectors. To demonstrate the advantages of wood current
ration. Decreasing the ratio of these nonactive materials in each collectors, an ultrathick LiFePO4 (LFP) electrode was prepared
of the components can effectively increase the energy density. by infiltrating LFP particles into the channels of the 3D current
The conventional way to prepare an electrode is through slurry- collector. In contrast, the conventional LFP electrode with a
casting the mixture (active materials, conductive additives, thickness of around 500 µm displays an easy deformability with
and binders) onto the metallic collectors (Figure 19a), where cracking and detachment from the current collector, which will
increasing the electrode thickness can reduce the percentage of result in a poor cycling stability. The as-prepared LFP in carbon
current collectors in batteries. Unfortunately, deformation and framework (LFP-CF) electrode delivered a high mass loading of
fracturing of electrode occurs upon the increase of electrode 60 mg cm−2 with a capacity of 7.6 mAh cm−2 (95 Ah L−1 based
thickness. Additionally, ionic transportation will be another chal- on volume) while the conventional LFP electrode can only
lenge when the electrode became thicker.[118] To maintain a fast exhibited about 4 mAh cm−2 (Figure 20b). Furthermore, the
transportation of ions and electrons, shortening the diffusion LFP-CF electrode with a thickness of 800 µm has shown great
distance by reducing the tortuosity in thick electrode can be an stress tolerance without cracking and detachment issues, which
effective way. According to the definition of tortuosity presented enable a more stable capacity retention at 2 mA cm−2.
as Equation (1)[119] To date, the commercially available LIBs in the market are
mainly employing lithium-metal oxide cathodes and graphite
τ = ε (D/DT ) (1) anodes. The energy density based on intercalation mechanism
Figure 19. a) Planar Cu foils as conventional current collectors in LIBs. b) A 3D current collector derived from carbonized wood enables a thicker
electrode for batteries. Reproduced with permission.[72] Copyright 2017, National Academy of Sciences.
Figure 20. a,b) Carbonized wood as current collector for Li-ion batteries. Reproduced with permission.[125] Copyright 2017, WILEY-VCH. c,d) Carbon-
ized wood as the S host for Li–S batteries. Reproduced with permission.[124] Copyright 2017, American Chemical Society.
is not high enough to meet the demands of electric vehi- RGO nanosheets can chemically bond with the intermediate
cles. Recently, lithium–sulfur (Li–S) batteries are becoming products of sulfur to locally trap them and prevent their migra-
a potential alternative to LIBs due to their much higher the- tion to the anode. The low tortuosity and open microchannels
oretical energy density (2567 Wh kg−1 for the Li–S battery vs can allow better electrolyte permeation through the composite
387 Wh kg−1 for the LiCoO2–graphite battery).[121] However, electrode (Figure 20c,d). The as-obtained electrode with a sulfur
issues including the insulating nature of sulfur and its lithi- mass loading of 7.8 mg cm−2 showed a high areal capacity of
ated products (Li2S and Li2S2), the high solubility of poly- 6.7 mAh cm−2 at a current density of 1.56 mA cm−2 and excel-
sulfides (Li2Sn, 3 ≤ n ≤ 6), and the well-known shuttle effects lent cycling stability (90% retention after 50 cycles). When the
have significantly hampered the development of Li–S bat- sulfur mass loading is increased to 21.3 mg cm−2, the electrode
teries. To address these issues, various carbon materials have can reach an even higher areal capacity of up to 15.2 mAh cm−2.
been used to host sulfur as a composite cathode, which show The facile but effective wood-inspired strategy for replacing
great promise.[122] In 2015, Kaskel and co-workers synthesized metallic current collectors can also be applied in many other
a hierarchically structured biomorphic carbide-derived carbon energy storage and conversion applications.[124]
(CDC) using natural wood as templates.[123] The as-prepared Benefiting from the advantages of being abundant, low-
hierarchical structured carbon materials exhibited longitudi- cost, lightweight, and renewable, nanocellulose-based mate-
nally orientated macropores, which were inherited from the rials can be employed in preparing lightweight and wearable
wood structure. Moreover, due to the activation process and electrodes.[126] For example, nanocellulose-based aerogels
CDC approach, well-defined and narrowly distributed micro- and foams were developed as lightweight 3D current collec-
and mesopores were obtained as well, which delivered specific tors for high mass loading of active materials, which improve
surface area (SSA) up to 1750 m2 g−1, pore volumes contribu- the energy density of the whole devices.[127,128] Enlightened by
tion from micro-/mesopores up to 1.0 cm3 g−1, and macropores this, Lee and co-worrkers designed a CNF/multiwalled carbon
of 1.2 cm3 g−1. After loading sulfur, the hierarchically struc- nanotube-based (CNF/MWNT-based) hetero-nanonet (HN)
tured carbon/S cathode exhibited stable performance, where a paper battery (Figure 21a).[128] The constructed 3D porous CNF/
capacity of ≈600 mAh gsulfur−1 at 20 mA cm−2 was delivered. MWNT networks enable the formation of both electron and ion
However, the conventional sulfur cathode was also prepared transport pathways in the CNF/MWNT-active powders (denotes
through the slurry-casting method, which would face the same as CM) electrodes, which can boost the electrochemical reac-
challenge during the preparation of thick electrodes. Recently, tion kinetics. Moreover, the CNF/MWNT-based electrodes are
Hu and co-workers engineered a sulfur cathode architecture metallic current collector free, which allows multiple stacking
based on carbonized wood, which can provide an ideal structure of CM electrodes in series to form ultrathick electrodes, largely
for high sulfur mass loading (S@C-wood).[124] The 3D carbon increasing the energy density. The assembled single-unit Li-ion
matrix (C-wood) is obtained by carbonizing and activating nat- battery based on the multilayered LiNi0.5Mn1.5O4 cathodes
ural wood that is cut perpendicular to its growth direction and (thickness: 450 µm) and graphite anodes (thickness: 160 µm)
then filled with reduced graphene oxide (RGO) nanosheets. (Figure 21b) exhibits a high energy density of 226 Wh kg−1 at
RGO serves as an electronically conductive network to enhance 400 W kg−1, which exceeds the index of long-range electrical
the electron transport, and the oxygen functional groups on vehicles (Figure 21b,c).
Figure 21. a) Schematic illustration showing the preparation process of the CM electrodes. b) Schematic illustration of the assembled single cell
based on the CM electrodes. c) Ragone plot of single-unit HN paper cells, where the gravimetric energy/power densities of cells were determined on
the basis of cell mass ( = cathode + anode + separator). a–c) Reproduced with permission.[128] Copyright 2015, WILEY-VCH. d) Schematic showing
the preparation process of the CNC–MWCNT aerogel. e) Photograph showing the prepared CNC–MWCNT aerogel. f) Schematic of the assembled
symmetric supercapacitor. g) Capacitance retention and Coulombic efficiency as a function of cycle numbers. The inset shows the initial and terminal
charge–discharge curves at a current density of 15 mA cm−2). d–g)Reproduced with permission.[133] Copyright 2016, WILEY-VCH.
The electrochemical capacitor (EC) is another type of advanced energy storage systems. However, since wood pos-
advanced energy storage device with high power density but sesses a unique hierarchical porous structure, how to utilize
low energy density. During the past decades, much effort the different sized pores well and infiltrate electrode materials
has been dedicated to improving the energy storage ability of uniformly into the channels remain challenges to be overcome.
EC for practical applications.[129] Fundamental research has To obtain a higher tap density, the conventional method for
focused on the exploration of the active materials, electrolytes, planar metallic foils is to press the as-prepared electrode under
and cell structure.[130] Meanwhile, new applications of wear- a high pressure, which will inevitably result in the fracture of
able electronics have generated much interest for the flexible carbonized wood.[73] The rigidity and brittleness are drawbacks
and compressible energy storage devices using cellulose-based that prevent wood materials from becoming a multifunctional
materials.[131] Several recent review papers have covered the current collector. Therefore, exploring various strategies and
progress in material preparation, electrode fabrication, device advanced technologies to improve the flexibility and enhance
configuration, and applications related to this topic.[2,132] Due the mechanical properties while maintaining high packing
to the limited space, here we briefly introduce a work from density is extremely critical. Moreover, a better understanding
Zhitomirsky and co-workers, where they reported a super about the diversity of porous structure from different types of
flexible and highly compressible electrode, of which polypyr- wood may be beneficial and necessary for follow-up studies.
role (PPy) is in situ polymerized in a cellulose-based current Optimizing the porosity of wood materials by various carbon-
collector.[133] The nanocellulose-based 3D current collector is ization treatments can be of great significance as well, which
prepared by facile solution-based freeze-drying, which has a shows great promise in potential applications beyond energy
density of 21 ± 3 mg cm−3 and large size (Figure 21d,e). Bene storage systems, such as adsorption, catalysis, and separation.
fiting from the 3D porous structure, the mass loading of the
CNC–MWCNT aerogels can be increased to 17.8 mg cm−2. Two
CNC–MWCNT aerogel electrodes with a PPy mass loading of 6.2. Biodegradable Energy Storage Devices
6.1 mg cm−2 were used to assemble symmetric supercapacitors
(Figure 21f). The assembled cell exhibited a capacitance reten- Growing environmental awareness throughout the world has
tion of 93.4% and 86.9% and Coulombic efficiency of 100% and stimulated material design toward greater compatibility with
93.3%, after 1000 and 5000 cycles, respectively (Figure 21g). the environment.[134] Beyond batteries, our group further
As discussed above, compared with traditional planar applied wood for supercapacitors with ultrahigh areal capaci-
metallic current collectors, wood and its derived materials tance and great biocompatibility.[73] The schematic illustration
shorten the diffusion pathway by low-tortuous channels, enable in Figure 22a shows the sandwiched wood-structured asym-
a fast transportation of electrons and ions, and boost the elec- metric supercapacitor, which contains an activated wood-
trochemical kinetics, which have shown great promise for carbon anode (basswood stabilized at 260 °C in air and then
Figure 22. a) Schematic illustration of the all-wood-structured supercapacitor and the corresponding photographs of individual components. b,c) Photo
graph and rate performance of all-wood-structured supercapacitor. Reproduced with permission.[73] Copyright 2017, the Royal Society of Chemistry.
carbonized at 1000 °C for 6 h in Ar), a thin wood membrane materials together and maintaining robust contact with the
separator and an MnO2/wood carbon cathode. The aligned current collector. Poly(vinylidene fluoride) (PVDF) and poly
channels are filled with aqueous electrolyte to let the ions travel tetrafluoroethylene (PTFE)-based binders are widely used in
through directly, enabling a sufficient contact with ion flux and LIBs.[135] However, PVDF and PTFE are hardly biodegradable
a fast-ionic transport, and further facilitating a good rate perfor- under natural conditions, which can lead to detrimental envi-
mance. Both the electrode and separator materials derived from ronmental issues. In contrast, with its excellent biodegradability
raw wood construct an all-wood-structure supercapacitor, exhib- and flexibility, CNF can be used as a type of green binder.[136]
iting a low-cost, environmentally friendly, and biodegradable Recently, Cornell and co-workers reported flexible positive
feature (Figure 22b). As displayed in Figure 22c, the all-wood and negative electrodes by using a small amount of TOCNF
super capacitor exhibited an extraordinary rate performance as binder (Figure 23a).[137] The galvanostatic charge–discharge
with a high areal capacitance of 3.6 F cm−2 at 1 mA cm−2 and curves of the flexible TOCNF-based positive electrodes with dif-
1.3 F cm−2 at 20 mA cm−2. By rationally utilizing the structural ferent ratios of active materials, carbon additives, and TOCNF
merits of natural/carbonized wood, this all-wood supercapacitor are shown in Figure 23b. The 88–7–5 (active materials–carbon–
delivers a high energy/power density (≈1.6 mWh cm−2 at TOCNF) electrode shows a high polarization. Even though
1044 mW cm−2) with a high areal mass loading of 75 mg cm−2 the polarization decreases with the improved carbon ratio
for the cathode, foreseeing the development of high-perfor- (86–9–5 and 84–11–5 electrodes), the specific capacity decreases
mance energy storage devices. as well. Additionally, the high mass loading of active material
Binder is a key component in electrode configuration, (87–9–4 electrode) can achieve a high specific capacity but the
which plays a critical role in holding the active and conductive polarization is still high. As a result, the 85–11–4 electrode with
Figure 23. a) Schematic illustration of the preparation process of the TEMPO-oxidized CNF (TOCNF)-based flexible electrodes. b) Galvanostatic charge/
discharge curves of the flexible paper-like electrodes with different ratios of LiFePO4 to Super-P carbon to TOCNF under a current density of 0.1 C.
c) Photograph showing the flexible cathode electrode. d) Photograph showing the assembled flexible battery based on the flexible TOCNF-based cathode
and anode. e) Photograph showing the flexible NFC-based paper electrode. a–e) Reproduced with permission.[137] Copyright 2016, American Chemical
Society. f) SEM image showing the cross section of the bilayered electrode. g) Galvanostatic charge/discharge curves of a bilayered electrode measured
against a lithium metal counter electrode over ten cycles at a current rate of C/10. f,g) Reproduced with permission.[138] Copyright 2013, Elsevier.
an optimized ratio can achieve the highest specific capacity by infusing metallic Li into C-wood framework.[72] A thin layer
and the lowest polarization. Figure 23c displays a photograph of ZnO was coated onto C-wood before molten Li infusion to
to demonstrate the flexibility of the cathode electrode. A bend- improve the affinity between carbon and Li, leading to fast infu-
able battery assembled with TOCNF-based cathode and anode sion of molten Li into ZnO-coated C-wood channels within
can light a blue LED (Figure 23d). Recently, Wågberg and co- 1 s. The morphology evolution of the C-wood, ZnO-coated
workers also reported a flexible bilayered NFC-based positive C-wood, and the as-formed Li/C-wood composite is clearly
electrode (Figure 23e).[138] The cross-sectional SEM image of presented in Figure 24b. The traditional commercial Li foils
the flexible electrode clearly reveals the bilayered structure. show unstable voltage profiles and larger overpotential with
This bilayered electrode shows a seamless contact between the irregular fluctuation at 3 mA cm−2, indicating that Li dendritic
LiFePO4 and carbon layers, which can enable favorable elec- growth occurs upon the repeated stripping/plating process. In
tron transport. The assembled cell using the TOCNF-based sharp comparison, the Li/C electrodes exhibited a flat voltage
cathode and lithium anode exhibits a superior specific capacity profile with a lower overpotential of 90 mV at 3 mA cm−2 and
of 151 mAh g−1 and excellent cycling performance. a superior cycling performance up to 225 cycles (Figure 24c).
Although the wood and wood-based materials used in Similarly, molten Na can be infused into C-wood as well. Inter-
energy storage devices, such as wood separator and CNF estingly, the infusion process did not require a ZnO coating.
binder, possess favorable biodegradability and biocompat- The bare Na electrodes show dramatic increase of voltage hys-
ibility, the active materials and conductive additives such as teresis after 50 h cycling at 1 mA cm−2.[145] However, by using
CNT are non-biodegradable, which still have a certain impact C-wood matrix, the Na-wood electrodes exhibit stable cycling
on the environment. Moreover, the wood has a high wet- performance for more than 500 h. The achieved extraordi-
expansion ratio and is easily destroyed by pests under moist nary stability of metallic anodes should be account for using
conditions, which can significantly decrease the stability and the aligned channel structure from C-wood. The channel walls
long-term usability.[139] For CNF, the conventional prepara- had a strong mechanical property and electrochemical stability
tion methods still suffer from high cost and complicated pro- that could accommodate the infinite volume change of metallic
cesses containing noxious chemicals.[3] Importantly, despite anodes upon repeated cycling. Generally, the inhomogeneous
the good degradability of CNF binder, its stability in aqueous metal ion flux accounts for the nonuniform metallic nucleation
solution needs to be further improved for meeting the long- and dendritic proliferation. Meanwhile, according to the Sand’s
term cycling requirement. Therefore, while ensuring good time proposed by Brissot et al., the metallic dendritic growth
electrochemical performance in energy storage devices, con- can be alleviated by decreasing the local current density.[146]
tinuous research on modification of wood and wood-derived Hence, the C-wood substrate with a large specific surface area
materials is necessary to obtain better stability and adjust the enables a minimized local current density, which effectively
biodegradability. inhibits the metallic dendrites and extends the lifespan of bat-
teries using metallic anodes.
The 3D electrode structure design inspired by wood has
6.3. Carbonized Wood as Host for High-Capacity been demonstrated to be an effective way to accommodate the
Metallic Anodes volume change and alleviate the dendritic growth of metallic
anodes, whereas, to fully solve the safety concerns for the com-
The metallic Li anode has been considered the “holy grail mercialization of metallic anodes, a combination of different
anode.”[114,140] Although metallic Li has the highest capacity approaches other than one single step is needed, such as opti-
and lowest potential, unfortunately, the realization of conven- mization of electrolyte compositions and battery configuration,
tional planar Li foil in practical applications is facing challenges modification of separator, adoption of strengthened artificial
including large volume variation, low Coulombic efficiency, and solid-electrolyte interface (SEI), and development of novel
safety concerns.[115,141,142] Recently, various solutions have been structure design.[117,141] A fundamental understanding of wet-
reported to improve the stability of metallic Li anode, such as ting mechanism at molten metal/C-wood interface should be
using 3D porous current collectors and encapsulation of Li in a further investigated.[72] As is known to all, the metallic anodes
matrix.[143] These continuous 3D or matrix networks with pores play a vital role in the development of high energy density bat-
have shown obvious alleviation of metallic dendrites and effec- teries, especially for pairing with nonlithiated cathode mate-
tive confinement for volume changes of metallic anodes upon rials such as sulfur and oxygen. To increase the energy den-
repeated cycling processes. sity of batteries, great effort is needed to focus on exploring
Different from the other porous frameworks, C-wood can reliable cathode material with comparable capacity and opti-
provide a unique vertical channel structure with low tortu- mizing full cell configuration. Besides, compared with the tra-
osity and high porosity along the growth direction, as dis- ditional manufacturing environment for batteries, the thermal
cussed in previous sections. The vertical channel walls create infusion process of molten Li needs to be conducted under
an expressway free of crossing junctions for electron transport. a critical environment with low humidity, pure inert atmos-
Furthermore, the moving Li ion flux in C-wood framework phere, and high-temperature tolerance, which demands the
is divided by each aligned channel wall and isolated horizon- manufacturers to further develop and improve the manufac-
tally within individual channels, which significantly limits the turing setup.
amplification of metallic deposition (Figure 24a).[144] According In summary, wood-based materials have made great
to the above-mentioned unique features from C-wood, Zhang advances in energy-related studies due to their unique natural
et al. reported a new strategy to achieve stable metallic anodes intrinsic structure and shown promising potential for the
Figure 24. a) Schematic illustration of the working mechanism of Li cycling on conventional planar Li foils and Li/C-wood electrodes as anodes in
Li batteries. b) Morphology evolution of C-wood, ZnO-coated C-wood, and Li/C-wood upon fabricating Li/C-wood composite electrode. c) Cycling
stability comparison of Li foils and Li/C-wood at 3 mA cm−2 with a capacity of 1 mAh cm−2. Reproduced with permission.[72] Copyright 2017, National
Academy of Sciences.
development of biodegradable, sustainable and high-energy- biodegradable and renewable characteristics, along with the
density energy storage devices. However, it is still urgent to high specific surface area and versatile surface chemistry, nano-
have a better understanding of the fundamental studies of cellulose has been widely applied in wastewater treatment. The
wood and its derived materials to achieve a high electrochem- applications of nanocellulose in wastewater treatment generally
ical performance. Moreover, improving industrial production include absorption/adsorption, catalytic degradation, and anti-
technologies with low cost is the key factor to realize the large- bacterial (Figure 25), and the specific applications span from
scalable and commercial applications of woody biomaterials for oil contaminant cleanup,[44,148] heavy metals’ adsorption,[149,150]
emerging energy storage devices. organic pollutant removal,[151] as well as antibacterial.[152] The
detailed applications of nanocellulose in wastewater treatments
have been recently reviewed,[153,154] and therefore will only be
7. Sustainable Application: Wastewater Treatment briefly outlined here.
Using nanocellulose as a bioabsorbent takes advantage of its
While enjoying the convenience brought by the fast industri- versatile surface chemistry as well as the tunable macroscopic
alization and economic growth, we are inevitably enduring forms that can facilitate post-treatment recovery and regen-
the deteriorated environment that comes along. Water pollu- eration. Cellulose aerogel, with 3D interconnected networks
tion has been one of the most pressing issues all around the as well as intact physical structures, has been widely adopted
world and the polluted water represents a significant threat as bioabsorbent in wastewater treatment.[43,44] Recently, Zhu
to human health. Many sources including urban runoff and et al. reported a facile method in fabricating hybrid aerogel
industrial wastewater contribute to the contaminants found containing CNC, carboxymethyl cellulose (CMC) and metal–
in water bodies, consisting of over 700 organic and inorganic organic framework (MOF), combining the respective advan-
pollutants as well as microbial populations.[147] Owing to its tages of hierarchical structure for nanocellulose and large
Figure 25. CNF aerogel for water treatment. a) CNC–CMC–MOF aerogel (1:1:1) containing University of Oslo-66 (UiO-66) and Materials Institute
de Lavoisier-100(Fe) (MIL-100(Fe)). (b) SEM image of aerogel with 50 wt% UiO-66. c) Photograph of the contaminated aqueous solution before
and after adsorption Cr(VI) in the aerogel with 50 wt% UiO-66. a–c) Reproduced with permission.[149] Copyright 2016, WILEY-VCH. d) Photograph
showing removal of a layer of Sudan IV red-dyed decane on a water surface by an organosilane-modified CNF aerogel. Reproduced with permission.[148]
Copyright 2014, the Royal Society of Chemistry. e) Schematic illustration of the formation mechanism of Au NPs@CNs for catalytic reduction of 4-nitro-
phenol. f) Time-dependent UV–vis spectra for the reduction of 4-NP catalyzed with Au NPs@CNs. e,f) Reproduced with permission.[156] Copyright 2014,
the Royal Society of Chemistry. g) UV–vis absorbance spectra of CNF–Ag NPs (black: pre-dialysis; gray: post-dialysis): inset: photographs of CNF–Ag
NPs before (left) and after (right) dialysis. h) TEM image of CNF Ag NPs after 18 h of incubation in LB media at 37 °C. i) Fluorescence microscopy image
of bacteria in the 150 × 10−6 m CNF–Ag NPs for 18 h at 37 °C. g–i) Reproduced with permission.[152] Copyright 2014, the Royal Society of Chemistry.
specific surface area and porosity for MOF (Figure 25 a,b).[149] membrane for catalytic degradation of organic compounds,
The hybrid aerogel was tested for Cr(VI) removal, converting a using methylene blue dye as a model compound (Figure 26a).[70]
light yellow solution containing potassium dichromate to color- The complex mesoporous wood structure provides optimal ver-
less, indicating successful removal of Cr(VI) from the solution tical channels for polluted water to pass through, but still allows
(Figure 25c). Due to the highly porous structure with porosity enough residence time for the organic compounds to contact
reaching 99.9%, CNF aerogel can store a significant amount of the catalyst on the inner cell walls. Due to the reducing power
liquid in the macroscopic pores.[43] Therefore, when being mod- of lignin, Pd nanoparticles can be reduced from PdCl2 solution
ified to increase hydrophobicity, the superabsorptive aerogel on the surface of wood cell walls, being captured and stabilized
can function as an efficient absorber for oil/water separation, by the polar functional groups (COOH, OH, CO) pre-
an essential step in removing oil contaminants from water sent in the cellulose, hemicellulose and lignin molecules. This
(Figure 25d). This organosilane-modified CNF aerogel showed successful reduction of Pd NPs on wood can be visualized from
an absorption capacity as high as 360 g g−1 toward chloroform, the black color, and once contaminated water flows through the
considerably higher than other types of polymeric aerogel channels of Pd NPs decorated wood membranes, the methylene
or foam. blue will be reduced to colorless molecules due to the catalytic
Catalytic decomposition of organic pollutants represents effect of Pd NPs (Figure 26b). This visual observation can be
another effective method for wastewater treatment, typically corroborated by the UV–vis absorption spectrogram, showing
employing inorganic nanoparticles such as photocatalytic or that the absorption peak from methylene blue disappeared after
noble metal nanoparticles.[154] As nanocellulose has high spe- treatment, indicating complete degradation of the compound
cific surface area and abundant surface functional groups, (Figure 26c). The degradation efficiency is stable throughout
such as hydroxyls, carboxyls, and carbonyls, it has been widely the pH range from 1 to 12 (Figure 26d), and at a water flow
used in the synthesis of noble metal nanoparticles, such as rate up to 1 × 105 L m−2 h−1 (Figure 26e). The turn over fre-
gold[155,156] and palladium nanoparticles[157] for catalytic degra- quency of our Pd NPs/wood membrane was determined to be
dation of organic compounds. CNCs have been found to serve 2.02 molMB molPd−1 min−1 at a rate of 1 × 105 L m−2 h−1, which
dual functions as both reducing agent and stabilizing template is significantly higher than that of other previously reported Pd
in the hydrothermal synthesis of gold nanoparticles.[156] The nanostructures.
surface hydroxyls can reduce HAuCl4 in 10 h, 120 °C hydro- The porous plant xylem has also been directly used as a nat-
thermal treatment to form gold nanoparticles (Au NPs) with an ural filter system to remove bacteria from drinking water.[158]
average size of 30.5 nm that can be stabilized by the oxygen- This filter showed a size cutoff of about 100 nm and over 99.9%
containing groups (COO−, OH) through complexing or of bacteria rejection. With a 1 cm2 filter under 5 psi pressure,
electrostatic interactions (Figure 25e). Catalytic degradation of it can deliver 4 L of drinking water per day, sufficient to meet
4-nitrophenol by CNCs supported Au NPs showed fast color the daily needs of one person. This high rejection rate of xylem
fade due to the reduction to 4-aminophenol, with 84.4% conver- is due to the pits that laterally connect the tracheids. Actually,
sion in 14 min, significantly higher than the unsupported Au the pit membrane contains nanoscale pores ranging from a few
NPs (Figure 25f). nanometers to a few hundred nanometers in living trees, which
Among various water pollutants, bacteria are one of the prevents air bubbles from crossing between tracheids. When
most deadly contaminating sources that has posed tremendous working as a water filter, it is the same pit membrane that pre-
threats to human health, especially in developing countries.[158] vents bacteria and dyes to pass through. Interestingly, when
Silver nanoparticles (Ag NPs), known for their antibacterial being dried, the plant xylem cannot function as a water filter as
properties, are prone to aggregate in physiological solu- the pit membrane can become irreversibly aspirated against the
tions,[159] and therefore are limited in performance. Stabilizing cell wall to block the water flow.
the as-synthesized Ag NPs with surface carboxylated CNF has 3D hierarchical structures, whether assembled from nano-
been reported, showing that Ag NPs remain uniformly dis- cellulose or directly from wood, are unique for wastewater treat-
persed on the CNF surface after incubating in Lysogeny broth ment in the following aspects. The tunable porous structure
(LB) media at 37 °C for 18 h, without signs of aggregation can function either as high flux flow channel or trap contami-
(Figure 25 g,h).[152] The CNF-stabilized Ag NPs showed 40% nant. Besides, the abundant surface functional groups of the
cell viability and 3log decrease in bacterial counts by measure of lignocellulosic components offer versatile organic or inorganic
the colony-forming unit value. Most interestingly, at sublethal chemistry for modification, deriving efficient wastewater treat-
level, extracellular polysaccharides were found to be secreted ment devices such as absorbent, filter, and catalytic reactors.
surrounding the bacteria, leading clusters of neighboring The abundant wood materials show great promise for low-cost
bacteria to precipitate out from the solution (Figure 25i). wastewater treatment instrumentation, and future researches
Although countless researches have been conducted using should be prioritized in the directions of introducing multi-
nanocellulose for wastewater treatment, the focus of the functionalities, enhancing treatment efficiency, reducing device
research has started to shift toward bulk wood for this pur- and maintenance cost, and large-scale production. However,
pose. The advantages of bulk wood for wastewater treatment to date, only limited applications have been investigated, and
are apparent, considering the natural hierarchical mesoporous wood-based materials with a broad spectrum of applications in
structures for water transport, abundant functional groups environmental remediation should be developed, to cover toxic
within the different compounds in the cell walls, as well as chemicals’ absorption, adsorption, degradation, and regen-
minimal physical and/or chemical processing. Recently, Chen eration. As an environment remediation device, it is critical
et al. reported direct fabrication of a palladium-decorated wood that no secondary contamination should be generated during
Figure 26. a) Schematic showing basswood decorated with Pd NPs for water treatment. b) Experimental setup for the water treatment tests with the
photograph and SEM images of Pd-NP-decorated wood membrane shown on the right. The blue solution consists of 30 mg L−1 methylene blue (MB)
and 100 mg L−1 NaBH4. c) UV–vis spectra of the MB solution before and after flowing through Pd NPs/wood membrane. d,e) The degradation efficiency
at different pH values (d) and concentrations (e) of the MB solution. The inset shows the turnover frequency of Pd NPs/wood membrane compared
to other Pd-based materials reported in the literature. Reproduced with permission.[70] Copyright 2017, American Chemical Society.
postfunctionalization of wood- or cellulose-based materials. For root xylem, and then transport the water upward to evaporate
example, to achieve hydrophobicity, the cellulose foams or aero- through leaves. Over 97% of water absorbed through the root
gels are commonly modified with fluorinated or organosilane system has been lost to the environment through transpira-
chemicals, which are generally hazardous or toxic to human tion.[163] Driven by the solar energy, tree transpiration and gut-
and environment.[43] Therefore, post-treatment and functionali- tation constitute an essential part for the global water cycle
zation should focus on green chemistry to avoid using of toxic system, serving as a natural model for solar energy utilization
chemicals and solvents. Additionally, beyond water treatment, and water purification.
environmental remediation should also be further expanded to As a vast and sustainable energy source, solar energy has
other areas including air and soil regeneration. been extensively explored in the generation of electrical[164] and
thermal energies.[165–167] Solar-driven evaporation is regarded as
an eco-friendly and sustainable technology for water purifica-
8. Sustainable Application: High-Efficiency Solar tion. However, the conventional evaporation strategies usually
Steam toward Water Desalination involve heating the bulk water under concentrated solar illumi-
nation, which suffer from inferior conversion efficiency. Con-
Fresh water scarcity is a severe global issue that continues sidering the feasibility and scalability, finding a cost-effective
to worsen due to population growth, climate change, and and scalable strategy to address the water scarcity issue has
increased farming practice.[160,161] Many areas around the world never been more pressing. The emerging solar steam genera-
suffer from severe water scarcity for at least 5 months of the tion is generally considered as an efficient water desalination
year, and two thirds of the global populations (≈ 4 billion) and purification technology, which can effectively solve the
have a severe water scarcity issue for at least 1 month of the water scarcity issue.[167–169] The ideal solar steam generator by
year (Figure 27).[161] Much effort has focused on searching for heat localization commonly has successive combinations of
efficient technological solutions to address this water scarcity sunlight absorption, thermal insulation, and water transporta-
issue.[162] Trees, as natural organisms that rely on water and tion parts. For the light absorption layer, it is expected to have
CO2 for photosynthesis, absorb underground water through a high broadband solar absorption and effective photothermal
Figure 27. Annual average monthly fresh water scarcity from 1996 to 2005. Reproduced under the terms of the CC-BY 4.0 license.[161] Copyright 2016,
The Authors, published by the American Association for the Advancement of Science.
transition. Favorable heat localization on the absorbing layer bilayered solar steam generator, which consists of natural
is necessary to reduce heat loss, and has been investigated by wood and graphene oxide (GO) as the light absorbing layer
adopting the solar steam generators with 1D and 2D water (Figure 28j).[173] The wood matrix perpendicular to the growth
paths.[165,170] With this design, water transport is confined in 1D direction possesses highly porous microstructure (Figure 28k).
and 2D porous paths, which can significantly suppress the heat The GO layer attaches tightly on the porous wood matrix, con-
dissipation, thus, improve the conversion efficiency. Addition- tributing to high solar absorption and photothermal conversion
ally, the thermal insulation part should have low thermal con- (Figure 28l). The bilayered wood-based solar steam generator
duction to suppress the heat loss to the bulk water. Favorable with porous structure, high light absorption, good hydrophi-
hydrophilicity and porous microstructure contributes to unhin- licity, and low thermal conductivity delivers a high evapora-
dered vapor escape. Additionally, the hydrophilic and intercon- tion rate of 14.02 kg m−2 h−1 under the solar illumination
nected porous structure is necessary to ensure a continuous of 12 kW m−2 (Figure 28m).
water supply for steam generation. Cellulose, derived from either biomass, such as woods, or
Inspired by tree transpiration, natural wood with open and microorganisms, such as bacteria, has several advantages of
aligned microchannels can be used for effective solar steam superb flexibility, good hydrophilicity, and excellent mechan-
generation.[171] Hu and co-workers recently reported a tree- ical properties—all favorable for stable solar steam generation.
inspired design concept of solar steam generation device based Recently, our group reported an all-in-one solar-steam-genera-
on a CNT-modified flexible wood (F-Wood/CNT) membrane tion device with a concave structure fabricated by layer-by-layer
(Figure 28a,b).[172] The coated thin CNT layer can absorb sun- 3D printing.[174] The all-in-one solar steam generator contains a
light effectively and localize the heat on the top surface due to porous CNT/GO top layer for solar energy absorption and fast
the excellent thermal insulation properties of the flexible wood. vapor escape, a underlying GO/NFC layer for restricting heat
Meanwhile, water can transport along the vertically aligned dissipation to the bulk water while wicking water upward to the
microchannels and up to the evaporating surface. The SEM top CNT/GO layer for steam generation, and porous GO/NFC
image of the top surface of the F-Wood/CNTs shows highly wall to continuously absorb water upward for sustained water
porous structure (Figure 28c), which can increase the light supply (Figure 29a). Moreover, the air trapped between GO/
reflection paths and maximally absorb the solar energy. The NFC walls can act as an effective thermal insulator to greatly
enlarged SEM image further reveals uniform CNTs’ coverage suppress thermal losses to the bulk water, leading to a highly
on the natural wood, responsible for efficient light absorption efficient solar steam generator. The porosity of the 3D-printed
(Figure 28d). The SEM image of the cross section displays the solar steam generator reaches up to 97.3% (Figure 29b).
numerous aligned microchannels, which can contribute to Despite its highly porous structure, this solar steam generator
unimpeded water transport (Figure 28e,f). The F-Wood/CNT shows good structural stability that can support 0.5 kg of weight
shows a high absorption of ≈98% in the visible and infrared without deformation.
regions, which is greatly higher than ≈20% for pure F-Wood During solar steam generation, light is absorbed through the
(Figure 2g). The evaporation rates under different illuminations top CNT/GO layer, heating up the water transported through
of 1, 3, 5, 7, and 10 kW m−2 are about 0.95, 2.88, 5.14, 7.65, the porous GO/NFC wall to generate steam vapor (Figure 29c).
and 11.22 kg m−2 h−1 (Figure 28h), with corresponding conver- Under 1 sun illumination (1 kW m−2), the surface temperature
sion efficiencies of 65%, 67%, 72%, 77%, and 81%, respectively of pure water increases slightly to ≈20 °C. For the 3D printed
(Figure 28i). The high solar conversion efficiency is attributed evaporator (denoted as 3D-CG/GN), the surface temperature
to the high light absorption, unimpeded fast water transport can increase to 36.5 °C and remain constant, due to the effec-
and low thermal conductivity for heat localization. The inherent tive thermal insulation by the air trapped between the walls
aligned microchannels and favorable hydrophilicity enable nat- (Figure 29d). The evaporation rate of the 3D-CG/GN increases
ural wood to be applied in many other fields of energy water rapidly within a few minutes and remains constant over time
nexus. Singamaneni and co-workers also reported a wood-based (Figure 29e), showing an evaporation rate and efficiency of
Figure 28. a,b) Schematic illustration of the solar steam generator made from CNT-coated flexible wood membrane. c,d) Top-view SEM images of
the F-Wood/CNTs membrane showing the hair-like surface with numerous flower-like microsheets. e,f) Cross-sectional SEM images of the F-Wood/
CNTs membrane showing the aligned microchannels. g) Light absorption spectra of the F-Wood and F-Wood/CNTs membranes. h) The evaporation
rates as a function of different solar concentrations. i) Conversion efficiency of the F-Wood/CNTs membrane under various illumination intensities.
a–i) Reproduced with permission.[172] Copyright 2017, WILEY-VCH. j) Schematic illustration of the preparation of wood−GO-based solar steam gen-
erator. k) SEM image of the top surface of the natural wood. l) SEM image of the top surface of the GO film. m) Evaporation rates of the wood–GO,
wood and pure water under solar illumination of 12 kW m−2. j–m) Reproduced with permission.[173] Copyright 2016, American Chemical Society.
Figure 29. a) Schematic illustration of the component of the 3D-printed solar steam generation. b) Specific weight change of the 3D-CG/GN after
fully saturated with water. The inset shows 0.5 kg weight on the evaporator, exhibiting the good mechanical property. c) Schematic illustration showing
solar steam generation process. d) Surface temperature change of the pure water and 3D-CG/GN versus irradiation time. e) Evaporation rate of the
pure water and 3D-CG/GN versus irradiation time. f) Conversion efficiency and evaporation rate comparison of pure water, 3D-CG and 3D-CG/GN.
a–f) Reproduced with permission.[174] Copyright 2017, WILEY-VCH. g) Schematic showing the preparation process of the RGO/BNC:BNC aerogel.
h) Photographs showing the top and bottom of the bilayer evaporator. i) Cumulative weight loss of water under 10 kW m−2 illumination versus irradia-
tion time. g–i) Reproduced with permission.[169] Copyright 2016, WILEY-VCH.
1.25 kg m−2 h−1 and 85.6%, respectively, indicating excellent wood contribute to high energy conversion efficiency. However,
solar-steam-generation performance (Figure 29f). there are still a few issues need to be addressed. The natural
Recently, Singamaneni and co-workers reported a novel solar wood, when soaked in water for a long time, will be gradu-
steam generator by using the bacterial nanocellulose (BNC)- ally decomposed by the bacteria.[175] Therefore, the stability
based bilayer aerogel structure (Figure 29g).[169] To form the of natural wood in high-humidity environments needs to be
bilayered structure, bacterial cellulose is directly secreted on further enhanced to meet the requirements of long-term uti-
the GO/BNC composite (Figure 29h). The black GO/BNC com- lization. Modification of natural wood to ensure long-term sta-
posite layer is used for solar absorption and steam generation bility without performance decay warrants continued research.
through heat localization at the evaporation surface. The porous For the nanocellulose, its high cost and complicated assembly
and hydrophilic BNC layer can absorb and form a continuous hinder its practical application on the large scale. Moreover, the
supply of water. Benefiting from the unique bilayered architec- long-term stability of nanocellulose in water still needs to be
ture, the BNC-based solar steam generator has a high evapora- enhanced to maintain the stable solar-steam-generation perfor-
tion rate of 11.8 kg m−2 h−1 under 10 kW m−2 (Figure 29i). mance.[46] Besides, it should also be noted that the salt accumu-
Wood, with a naturally occurring porous hierarchical struc- lation in the evaporator based on the wood and wood-derived
ture, can be directly employed as a solar steam generator. The materials during the solar desalination is not yet evaluated.
numerous aligned microchannels, low thermal conductivity, The gradual salt accumulation in the solar steam generator will
and good hydrophilicity and mechanical properties of natural block the water pathways and illuminated area, which severely
decreases the solar desalination performance. Therefore, appro- short-term period. Therefore, sustainable application of wood-
priate material and structure design for effectively avoiding based materials requires continuous research in the aspects of
the salt accumulation during solar desalination is important to lowering material cost, enhancing performance, broadening
maintain the stable solar-steam-generation performance. applications, and efficient utilization of otherwise low-value
wood products, by overcoming some of the critical challenges.
First, the wood-based materials have to be economically
9. Conclusions and Perspectives competitive to their man-made competitors. From the aspect of
nanocellulose, cost has consistently existed as a real hurdle for
With increasing anxiety surrounding the depletion of natural its mass production and commercialization, due to the exten-
resources and deterioration of the environment, more atten- sive chemical and energy consumption during defibrillation
tion has been directed to sustainable development, in order to and assembly. It has been estimated that the cost of nanocel-
preserve our planet for future generations. With its vast and lulose can be as high as over 3000 USD per kg,[176] Therefore,
renewable raw material supply, the forest can provide us with future research should focus on reducing the production cost
materials that can be used in nearly every aspect of our daily life by finding more efficient extraction methods, such as new pre-
to replace unsustainable and energy-intensive man-made mate- treatment solvents, recyclable catalysts, less water consump-
rials. Switching to environmentally friendly, renewable, and tion, and low-energy requirements. The recent advances that
sustainable wood-based raw materials has attracted tremendous directly use wood via top-down approaches, instead of the com-
interest, and significant progress has been made in designing plicated isolation and assembly of nanocellulose, have inspired
wood-based hierarchical structures. Based on the starting mate- a more efficient and economical way to fabricate wood-based
rials, two opposite design strategies have been applied and functional materials. However, very limited research progress
summarized here, including the bottom-up assembly from has been reported and continuous developments are needed to
nanocellulose building block and top-down functionalization achieve scalable production and greater functionality.
from bulky wood blocks. These multifunctional hierarchical Second, the limited functionality of wood and cellulose
structures show great potential applications toward sustain- requires additional surface treatment and functionalization for
ability, in the proposed area to replace plastic, glass, and metal, advanced applications in the areas of energy storage and envi-
as well as to fabricate sustainable energy storage and water ronmental remediation. It should be noted that the principles
treatment devices. However, there is still a long way ahead to of green chemistry practice should be followed in the treatment
convert these promising concepts into a vision of a fully sus- process, to avoid secondary contamination to the environment.
tainable dreamland, as depicted in Figure 30, where all essen- Third, mechanical performance is an essential characteristic
tial housing supplies could be provided from a single tree. for more practical implementation of these wood-based mate-
The road to sustainability is never straightforward, as rials, especially as building materials. Although these newly
numerous technical challenges, economic and environmental developed wood-based materials, either in the form of fibers
concerns are inhibiting the development of sustainable wood- or films, have shown to exceed the performance of steel in the
and cellulose-based materials to ultimately compete with any aspect of specific mechanical properties (strength and mod-
of the successful synthetic materials. Although this will even- ulus normalized by the respective density) thanks to the much
tually benefit future generations, investigations into sustain- lower density of wood-based materials (approximately one
able wood- and cellulose-based materials to potentially replace order of magnitude lower than steel); the absolute mechanical
synthetic man-made counterparts may not benefit in any properties are significantly lower compared to these structural
Figure 30. A sustainable living environment that relies on wood-based materials for both construction and functional applications, with the ultimate
goal being to replace the unsustainable plastic, glass, and metals resources currently used in nearly all aspects from housing to water and energy
supplies.
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Wood-Based Nanotechnologies toward Sustainability

to alleviate our reliance on petroleum-based

replace nondegradable plastic, glass, and metal in electronics,

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