1 s2.0 S0079642522001062 Main - 2

Progress in Materials Science 132 (2023) 101025
Contents lists available at ScienceDirect
Progress in Materials Science

journal homepage: www.elsevier.com/locate/pmatsci
Transparent wood-based functional materials via a

top-down approach
Sailing Zhu a, 1, Subir Kumar Biswas b, 1, Zhe Qiu c, d, Yiying Yue f, Qiliang Fu a, e, *,
Feng Jiang c, *, Jingquan Han a, *
a
Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and
Materials, Joint International Research Lab of Lignocellulosic Functional Materials, College of Materials Science and Engineering, Nanjing Forestry
University, Nanjing 210037, China
b
Laboratory of Active Bio-Based Materials, Research Institute for Sustainable Humanosphere (RISH), Kyoto University, Uji, Kyoto 611-0011, Japan
c
Sustainable Functional Biomaterials Laboratory, Department of Wood Science, The University of British Columbia, Vancouver, BC V6T 1Z4,
Canada
d
Key Laboratory of Bio-based Material Science and Technology (Ministry of Education), College of Material Science and Engineering, Northeast
Forestry University, Hexing road 26, Harbin 150040, China
e
Scion, 49 Sala Street, Private Bag 3020, Rotorua 3046, New Zealand
f
College of Biology and Environment, Nanjing Forestry University, Nanjing 210037, China
A R T I C L E I N F O A B S T R A C T
Keywords: Transparent wood-based materials (TWMs), made by either bottom-up or top-down strategies,
Transparent wood have attracted great attention owing to their transparency, sustainability and multifunctionality.
Delignification Compared with materials prepared by a traditional bottom-up method, TWMs fabricated via a
Wood modification
top-down approach are promising as the natural hierarchical structure of wood is preserved with
Top-down approach
a high production efficiency, energy savings and scalability. Wood nanotechnologies, various
Structure and property
Functionalization and application chemical treatments and polymer impregnation or densification techniques have been developed
to fabricate TWMs, including transparent wood and transparent wood films, sharing similar
sustainability and optical transmittance while also preserving some uniqueness in applications
and compositions. Herein, we systematically provide an up-to-date summary on the state-of-the-
art for transparent wood and transparent wood films, with a special highlight on the proc
ess–structure–property–application perspective, establishing the combination of wood science,
material chemistry and physics with new horizons in TWM science. The integrated topics of
Abbreviations: TWM, transparent wood-based material (fabricated via top-down approach); TW, transparent wood; TWF, transparent wood film;
BWS, bleached wood scaffold; CNF, cellulose nanofibril; e-skin, electronic skin; NW, natural/native wood; UV, ultraviolet; UVA, ultraviolet A; UVB,
ultraviolet B; UVC, ultraviolet C; UPF, UV protection factor; MA, maleic anhydride; IA, itaconic anhydride; SA, succinic anhydride; PMMA, poly
methyl methacrylate; PVA, poly (vinyl alcohol); PVP, polyvinylpyrrolidone; PLIMA, poly(limonene acrylate); MF, melamine formaldehyde; TEMPO,
2,2,6,6-tetramethylpiperidinyl-1-oxyl; ATO, antimony-doped tin oxide; AgNW, silver nanowire; LED, light-emitting diode; ACEL, alternating current
electroluminescent; PET, polyethylene terephthalate; WLED, white light-emitting diode; FA, formaldehyde; ML, middle lamella; P, primary wall; S1,
outer layer; S2, middle layer; S3, inner layer; L-wood, transparent wood along the longitudinal direction; R-wood, transparent wood in the transverse
direction; PEAG, phosphate ester-polyethylene glycol; PDES, polymerizable deep eutectic solvents; CDs, carbon dots.
* Corresponding authors at: Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for
Forest Chemicals and Materials, Joint International Research Lab of Lignocellulosic Functional Materials, College of Materials Science and Engi
neering, Nanjing Forestry University, Nanjing 210037, China.
E-mail addresses: qiliang.fu@njfu.edu.cn (Q. Fu), feng.jiang@ubc.ca (F. Jiang), hjq@njfu.edu.cn (J. Han).
1
Equal contribution to this work.
https://doi.org/10.1016/j.pmatsci.2022.101025
Received 26 February 2022; Received in revised form 4 September 2022; Accepted 23 September 2022
Available online 3 October 2022
0079-6425/© 2022 Elsevier Ltd. All rights reserved.
S. Zhu et al. Progress in Materials Science 132 (2023) 101025
TWMs emphasize the relationship between nanostructure and properties. The structural and
functional design concepts are described for engineering production purposes. The emerging
applications of TWMs are also discussed for the potential replacement of glass and petroleum-
based plastics. Finally, an outlook and challenges are proposed for the future potential of func
tional TWMs in engineered production.
1. Introduction
With the rising demand for energy and environmental conservation, eco-friendly materials are desired to replace petroleum-based
materials for sustainable development [1–3]. Natural wood (NW) has been widely used for tools, furniture and buildings over the past
thousands of years, owing to its wide availability, environmentally friendly characteristics, low thermal conductivity, ease of pro
cessing and high specific strength [4–11]. Recently, nanotechnologies have been developed to modify and functionalize wood
structures at both the nanoscale and molecular levels, as well as to design wood-based functional materials [12–17]. The micro
structure of wood can be precisely manipulated to introduce additional functionalities by chemical or physical modifications, which
can further extend the applications of wood-based composites in areas including water treatment [18–23], energy harvesting [24–28],
energy storage [29–38], electronic and optical applications [39–48], nanofluidic and hydrogel devices [49–54], and fire retardancy
[55]. Among various wood-based products, transparent wood-based materials are promising bio-based composites with high trans
parency, low thermal conductivity and multifunctionalities [56–59]. These materials have promise in activities seeking the use of more
sustainable materials in emerging applications, such as energy-saving buildings, smart windows and optoelectronic devices [60–67].
Transparent wood-based materials can be prepared through either bottom-up or top-down approaches [15,68]. In the following
content of this review, all the transparent wood-based materials fabricated via a top-down approach are specially designated as TWMs.
In the bottom-up approach, materials are built from nanocellulose building blocks into thin films or bulk materials (e.g., aerogel and
hydrogel) [69–72]. Nanocellulose is disintegrated from tree, cotton, linen or bacteria cellulose by mechanical, chemical or biological
methods and can be further assembled into a cellulose nanofiber network [73–85]. In 2005, Yano et al. reported the fibrillation of
wood pulp into cellulose nanofibril (CNF) bundles via a mechanical disintegration process, followed by the assembly of nanofibrils to
create a transparent film, which exhibited a promising reinforcement effect for optically transparent composites [86]. On the other
hand, the top-down approach can directly convert NW into transparent wood or transparent thin films with excellent mechanical and
optical properties [87–89]. A porous bleached wood scaffold (BWS) can be prepared by chemically removing lignin and/or hemi
cellulose from wood cell walls. The BWS is then impregnated by polymers with a refractive index similar to that of cellulose or
densified, fabricating transparent wood (TW) or a transparent wood film (TWF), respectively.
Constructing nanocellulose into transparent thin films based on a bottom-up approach has been thoroughly reviewed
[60,62,64–65,90–94]. Isotropic transparent nanocellulose films can be fabricated by vacuum filtration of nanocellulose colloidal
suspensions followed by resin impregnation, demonstrating excellent properties including high flexibility, superb mechanical and
optical properties, and low thermal expansion efficiency [60,95]. These attributes make nanocellulose-based transparent films
favorable substrates for many emerging applications in optoelectronics, photonics and electronics (e.g., sensors, organic light-emitting
diode displays and energy storage devices) [47–48,60,62,64–65,90,96–104]. In addition, CNFs can be chemically modified or com
bined with inorganic nanoparticles/organic moieties, generating additional functionalities such as hydrophobicity, magnetic per
formance, electrical conductivity, fire retardancy and luminescence [105–110]. Although the size of the CNFs and the structure of the
cellulosic films are controllable, the mechanical performances of these isotropic films are suboptimal. To enhance their mechanical
strength, transparent nanocellulose films with anisotropic structures have been intensively studied to uniaxially align CNFs to improve
mechanical properties via mechanical stretching and electric/magnetic field alignment [111–119]. In recent years, these topics have
been summarized in many review articles [120–121]. However, the production of either isotropic or anisotropic nanocellulose films
using the bottom-up method requires relatively complex processes and consumes tremendous amounts of energy, chemicals, water and
time. Moreover, the scalability of functional nanocellulose materials via the bottom-up strategy is challenging.
Alternatively, a top-down approach demonstrates great promise in preparing large-scale transparent wood-based products, which
can facilely overcome the scale-up issue as this strategy starts with NW and ends up with a bulk material [122–124]. The top-down
approach can bypass nanocellulose isolation and reconstruction processes, which are considered the most time- and energy- inten
sive steps of the bottom-up method. For example, both TW and TWFs have been reported to be directly obtained from bulk wood
[87–89]. The cell walls of these materials with highly oriented cellulose are preserved, resulting in excellent mechanical properties.
More importantly, the preparation of TWMs is much easier, consuming less energy, chemicals, water and time than the bottom-up
approach. Although TW and TWFs are mainly composed of cellulose and directly converted from wood, they are theoretically
different materials in terms of three aspects. 1) Microstructure. TW maintains the honeycomb-like structure of wood cells, while TWFs
are completely densified, with a compact mortar-and-brick structure. 2) Chemical components. TWFs are polymer matrix-free ma
terials with pure holocellulose. However, the impregnation of refractive-index-matched polymers is necessary in the fabrication of TW,
which means that the main components of TW are holocellulose and infiltrated polymers. 3) Transparency mechanism. The refractive-
index-matched phases of TW allow light transmission through the composite material, whereas photons travel through TWFs as the
defects between air and holocellulose are removed by densification. Therefore, TW and TWFs (both defined as TWMs) are considered
two different wood-based materials in this review.
The top-down method is a promising and straightforward strategy that has prompted scientists to demonstrate multifunctional
2
Fig. 1. A brief summary of the inspiration and research progresses of TWMs, it is presented according to the timeline. Inspiration images.
Reproduced with permission [87]. Copyright 2012, Royal Society of Chemistry. Functional & structural TW image (left): Reproduced with
permission [89]. Copyright 2016, Wiley-VCH. Functional & structure TW image (right): Reproduced with permission [88]. Copyright 2016,
American Chemical Society. TW and Light management images: Reproduced with permission [125]. Copyright 2016, Elsevier. Energy efficient TW
image: Reproduced with permission [61]. Copyright 2016, Wiley-VCH. Luminescent TW image: Reproduced with permission [126]. Copyright
2017, Wiley-VCH. Luminescent & magnetic TW image: Reproduced with permission [127]. Copyright 2017, American Chemical Society. Heat-
shielding TW image: Reproduced with permission [128]. Copyright 2017, Royal Society of Chemistry. TWF image: Reproduced with permission
[115]. Copyright 2017, Wiley-VCH. Transparent plywood image: Reproduced with permission [129]. Copyright 2018, Elsevier. Large-thickness TW
image: Reproduced with permission [130]. Copyright 2018, Royal Society of Chemistry. Electrochromic device image: Reproduced with permission
[63]. Copyright 2018, Wiley-VCH. Flexible & conductive TW image: Reproduced with permission [131]. Copyright 2018, Royal Society of
Chemistry. Low haze TW image: Reproduced with permission [66]. Copyright 2019, American Chemical Society. Photochromic TW image:
Reproduced with permission [132]. Copyright 2019, Royal Society of Chemistry. ACEL device image: Reproduced with permission [133]. Copyright
2019, American Chemical Society. Heat-storage TW image: Reproduced with permission [134]. Copyright 2019, American Chemical Society. TW
solar cell image: Reproduced with permission [135]. Copyright 2019, American Chemical Society. Aesthetic TW: Reproduced with permission
[136]. Copyright 2020, Springer Nature. Flame-retardant TW image: Reproduced with permission [137]. Copyright 2020, Elsevier. Flexible TWF
sensor image: Reproduced with permission [138]. Copyright 2020, American Chemical Society. Luminescent TWF image: Reproduced with
permission [139]. Copyright 2020, American Chemical Society. TW gas sensor and TW white light-emitting diode (WLED) images: Reproduced with
permission [140]. Copyright 2020, American Chemical Society. Patternable TW image: Reproduced with permission [124]. Copyright 2021,
American Association for the Advancement of Science. Coloured TW image: Reproduced with permission [141]. Copyright 2021, American
Chemical Society. Shape-memory TW image: Reproduced with permission [142]. Copyright 2021, Elsevier. Fully bio-based TW image: Reproduced
with permission [143]. Copyright 2021, Wiley-VCH. TW e-skin image: Reproduced with permission [144]. Copyright 2021, Elsevier. Photon
diffusion in TW image: Reproduced with permission [145]. Copyright 2022, Wiley-VCH. Smart packaging TW: Reproduced with permission [146].
Copyright 2022, Elsevier.
3
TWMs in terms of material design concepts and functionalization routes [12]. Although recent progress on TW has been summarized
[57–58,147–149], TWFs made from top-down approaches have not yet been overviewed. Herein, the state-of-the-art TWMs are
systematically overviewed, including TW and TWFs, as shown in Fig. 1. In particular, this is the first time that TWFs have been
reviewed to the best of our knowledge. The materials science of the process–structure–property–application relationship is discussed.
This consists of applying material chemistry and nanotechnology to tailor the wood chemical structures (lignin removal and modi
fication), considering nanomorphologies (generation of meso- and/or nanostructures) and adding new functionalities (electrical
conductivity, fire retardancy, thermal insulating and optical properties) to TWMs. TWMs are discussed as potential replacements of
traditional glass and fossil-based plastics in emerging applications. Finally, we highlight some opportunities and challenges in the
engineered production of functional and sustainable TWMs.
2. Transparency mechanism and processing methods
NW is opaque under visible light due to light scattering and reflection at the interface between cell walls and lumens, as well as the
strong light absorption by wood tissue. Approximately 80 ~ 95 % of the light absorption in wood is due to the chromophores associated
with lignin and some extractives [152]. Lignin units have complex chromophores (e.g., carbon–carbon double bonds conjugated with
aromatic rings) that are responsible for the brownish color and light absorption in NW [15,153]. It has been reported that the refractive
indices (n) of lignin, hemicellulose and cellulose are 1.61, 1.53 and 1.53, respectively [154]. The multiscale porous structural com
bination of micro, meso- and macropores leads to much light scattering because of mismatched refractive indices at the boundaries
between the air-filled (n = 1.0) lumen spaces and cell walls (average n≈1.56) [57,155]. To achieve TWMs, two main steps are
necessary: removing the light-absorbent components (including removing and modifying lignin) and eliminating the mismatched
refractive index in the BWS (average n≈1.53) [88]. In terms of reducing the differences in the refractive index of the TWM, there are
two strategies via the top-down approach (Fig. 2a): 1) impregnating refractive index-matched polymers into BWSs and 2) densifying
BWSs into transparent thin films.
Fig. 2. (a) Schematically illustrate the fabrication of TW and TWFs: Reproduced with permission [150]. Copyright 2019, Elsevier. SEM image of
TW: Reproduced with permission [130]. Copyright 2018, Royal Society of Chemistry. SEM image of TWF: Reproduced with permission [138].
Copyright 2020, American Chemical Society. SEM images of cell wall structures of (b) NW, (c) delignified BWS, and (d) lignin-retaining BWS. The
insets are low-magnification SEM images. Red arrows point to the middle lamella-rich region in lignin. (b-d) Reproduced with permission [151].
Copyright 2017, Wiley-VCH.
4
The preparation of a BWS generally starts from removing or modifying the lignin from NW. A range of different chemical treatment
processes, such as delignification (lignin removal) and removal of the chromophores in lignin (lignin modification), are used
[68,156–160]. It is crucial to manipulate nanostructured wood by precisely controlling its nanopores in the cell walls through these
chemical treatments and process conditions (i.e., treatment time, the concentration of chemical solutions, pH value, and temperature).
Acidic sodium chlorite (NaClO2) treatment is commonly used for delignification. NW is mildly treated using 1 ~ 5 wt% NaClO2
aqueous solution in acetate buffer solution with a pH of 4.6 for 6 ~ 18 h (depending on the size and cutting direction of the sample)
[88,133,135]. As a result, most lignin is removed from the cell walls, especially in the lignin-rich middle lamella, resulting in the
creation of microscale and nanoscale pores (Fig. 2c). The original honeycomb structure of NW is preserved in the BWS (Fig. 2b).
NaClO2 generates unstable chlorous acid in acetate buffer solution, which can be further decomposed into chlorine and chlorine di
oxide to react with lignin by methods including oxidation of the phenolic structure and/or phenoxyl-radical ring opening [161–162].
The lignin content of balsa wood decreased from 24.9 to 2.9 wt% due to the breakdown of lignin carbohydrate complexes [88]. A
Fig. 3. (a) The hierarchical structure of wood from the tree to the cellulose molecule chain. Tree image: Reproduced with permission [215].
Copyright 2021, Wiley-VCH. Transverse section image: Reproduced with permission [155]. Copyright 2016, American Chemical Society. Vascular
tissue, Microfibril bundle, Elementary fibril and Cellulose chain images: Reproduced with permission [122]. Copyright 2020, Springer Nature. Cell
wall image: Reproduced with permission [12]. Copyright 2018, Wiley-VCH. (b) The photograph and morphology of TW. TW image: Reproduced
with permission [89]. Copyright 2016, Wiley-VCH. The center SEM image: Reproduced with permission [143]. Copyright 2021, Wiley-VCH. The
right SEM image: Reproduced with permission [129]. Copyright 2018, Elsevier. (c) The photograph and morphology of TWF. Reproduced with
permission [138]. Copyright 2020, American Chemical Society.
5
Table 1
S. Zhu et al.
Optical properties (550 nm), mechanical performances and thermal properties for TWM.
Sample Wood Thickness Density [g Wood (cellulose)a Optical Mechanical Thermal Ref.
species [mm] cm¡3] [vol%]
trb haze E σ ε [%] toughness [MJ/ tcc [W/m dd
[%] [%] [Gpa] [Mpa] m¡3(¡|-)] K¡1]
Delignified/PMMA Beech 0.1 70 2.5 150 ~10 [218]

0.3 30 18
0.6 18 40
0.7 15 49
Delignified/PMMA/PEG Birch 0.5 84 74 [134]
1.5 68 77 ~14.9 ~70.5 0.3
Delignified/PMMA Balsa 0.7 90 ~48 [88]
3.7 40 ~80
1.2 (5) 85 ~70 ~2.05 38 ~2.2
1.2 (19) 78 ~75 ~3.59 ~90.1 ~3.8
1.2 (65) 34.6 ~78
Delignified/PMMA Birch 1.3 25 70 70 19 270 [219]
Haze wood/epoxy Basswood (0.7) 18.4 (14.7) 90 80 ~76.36 ~2.21 ~0.87 0.24 // [66]
(0.7) 18.4 (14.7) ~14.60 ~1.88 ~0.13 ⊥
Clear wood/epoxy Basswood (0.7) 2.9 (2.5) 92 10 43.39 19.14 ~6.1 0.35 //
(0.7) 2.9 (2.5) 33.29 16.3 ~3.96 ⊥
Delignified/LIMA Balsa 1.2 12 87 46 [143]
SA esterified/ delignified/ Balsa 1.2 12 89 41
LIMA
Delignified/LIMA Balsa 2.0 12 80 62
6
LIMA
Delignified/LIMA Balsa 3.0 12 71 65
LIMA
Delignified/LIMA Birch 0.7 26 88 49 12.6 146.6 1.2
SA esterified/ delignified/ Birch 0.7 26 92 44 17.3 173.6 1.0
LIMA
Delignified/PMMA Balsa 2.0 70.6 76.3 4.8 41.4 // [182]
2.9 11.4 ⊥
MA esterified/ delignified/ Balsa 2.0 79.5 73.6 4.3 46.2 //
PMMA

3.1 18 ⊥
IA esterified/ delignified/ Balsa 2.0 76.6 76.2 4.3 54.9 //
PMMA
3.3 33.2 ⊥
SA esterified/ delignified/ Balsa 2.0 83.8 66.9 4.5 61.7 //
PMMA
2.9 12.8 ⊥
Delignified/PMMA Balsa 1.5 83 70 [130]
Acetylated/ delignified/ Balsa 1.5 5 92 50 4 78.9 ~ 2.2 1.0
PMMA
Delignified/epoxy Basswood (3) 90 2.37 45.38 1.2 // [89]
(3) ~80 1.22 23.38 0.59 ⊥
Delignified/PMMA Balsa 0.8 12 ~95 ~60 ~4.3 ~62.5 1.5 // [129]
0.8 12 ~2.4 ~14.6 0.7 ⊥
(continued on next page)
Table 1 (continued )
Sample Wood Thickness Density [g Wood (cellulose)a Optical Mechanical Thermal Ref.
S. Zhu et al.
species [mm] cm¡3] [vol%]
trb haze E σ ε [%] toughness [MJ/ tcc [W/m dd
[%] [%] [Gpa] [Mpa] m¡3(¡|-)] K¡1]
Ply 0/90/0/-90/ Balsa 3.5 10 83 80 ~4.1 ~50.1 1.2 //

0 delignified/PMMA
3.5 10 ~3.9 ~44.9 1.3 ⊥
Ply 0/45/90/-45/ Balsa 3.5 10 75 80 ~3.9 ~45.4 1.2 //
0 delignified/PMMA
3.5 10 ~3.5 ~42 1.4 ⊥
Delignified/PMMA Basswood 1.6 66 ~85 ~14.4 ~131.6 // [220]
1.6 ~3.43 ~9.11 ⊥
Acetylated/ delignified/ Basswood 1.6 72 ~79 ~12.0 ~72.7 //
PMMA
1.6 ~3.75 ~11.49 ⊥
Ply delignified/PMMA Basswood 3.2 ~90 6.7 75
Ply acetylated/ delignified/ Basswood 3.2 ~88 6.8 42
PMMA
Delignified/epoxy Balsa 2 77 ~69.13 // [221]
2 ~6.06 ⊥
Basswood 2 64 ~75.12 //
2 ~8.17 ⊥
Clear wood/PVA Balsa 0.8 91 15 ~3.85 ~143 4.2 ~3.03 ~0.39 // [67]
0.8 ~3.10 ~67 3.7 ~1.06 ~0.19 ⊥
Delignified/PMMA Balsa 1.5 86 68 [151]
Lignin-retaining/PMMA Balsa 1.5 83 75 ~100.7 ~2.18
Delignified/thiol − ene Balsa 1.2 ~5.0 85 63 3.2 53.7 2.1 [184]
7
Lignin-retaining/thiol − Balsa 1.2 ~4.3 90 36 3.4 59 2.5

ene
Lignin-retaining/UV resin Balsa 46.7 95.2 0.678 38.32 [222]
Compressed lignin- 80.8 66.7 2.276 113.75
retaining/UV resin
Delignified/PEAG Balsa 20 93 98 2.2 153.6 // [200]
Delignified/epoxy Poplar 0.09 89.4 // [198]
TWF Basswood 0.05 (0.46) ~1.40 ~90 ~86 [223]
TWF Basswood 0.08 (0.4) 90 350 23.2 7.38 [115]
TWF Balsa 0.055 (1) ~1.20 80 85 49.9 469.9 // [138]
0.1 ~74
0.14 ~70

0.2 ~60
TWF Balsa 0.06 (1) ~1.20 81 42.7 393.8 // [139]
0.06 (1) 5.7 76 ⊥
Luminent TWF 0.075 (1) 70 24.4 292 //
Luminent TWF 0.075 (1) 5.3 64 ⊥
TWF Balsa 0.08 (2) ~1.32 80 70 ~51.1 ~449.1 1.75 [191]
TWF Balsa 0.06 ~1.24 77 73.5 426 [189]
TWF Balsa 0.055 ~1.25 24.54 196.8 // [224]
0.055 10.97 37.93 ⊥
The‖symbol represents the light/applied stress/transferred heat along the wood channel direction. The⊥symbol represents the light/applied stress/transferred heat perpendicular to the wood channel
direction.
a
The wood volume fraction denotes the sum of the volume fractions lignin, hemicellulose and cellulose (the cellulose volume fraction refers to the volume fraction of cellulose);
b
tr refers to transmittance;
c
tc refers to the thermal conductivity;
d
d refers to the direction.
similar study using sodium hypochlorite (NaClO) was reported by Fink in 1992 [154]. During the delignification treatment, oxidation
and chlorination reactions attacked the benzoquinone structure and the conjugated double bond of the side chain in lignin, leading to
dissolution of lignin in water. A pulping method using alkaline sodium sulfite (Na2SO3 + NaOH) was reported by Hu’s group [89].
Under alkaline cooking conditions, sulfite, bisulfite and hydroxide ions interacted with lignin carbohydrate complexes, enabling the
cleavage of ether bonds [163]. An additional hydrogen peroxide (H2O2) bleaching process was performed, resulting in a lignin content
of less than 3 wt%. In another strategy, peracetic acid or glacial acetic acid/H2O2 solution can selectively remove lignin [55,164–165].
Hydroxonium ions generated from peroxy bonds can attack the electron-rich positions in lignin (olephinic side chain and benzene
ring), resulting in the cleavage of water-soluble lignin [161]. Although several other delignification treatments have also been carried
out (e.g., ionic liquid, deep eutectic solvent or biological enzyme treatments) [166–176], the delignification mechanism of these
treatments is still unclear and needs further investigation.
Unlike the lignin-removal method, the lignin-modification method does not extract lignin but rather changes its structure and
simultaneously removes chromophores. Jungstedt et al. established a suitable analysis method to combine digital image correlation
and a finite element model for the investigation of the fracture toughness of transparent wood [177]. The results show the nonlinear
localized strain and stress development in the cohesive zone. The removal of lignin results in substantially inferior bulk wood structural
properties, since lignin acts as a binder that cross-links holocellulose and the weakened delignified middle lamella facilitates crack
growth [177]. Moreover, during delignification processes, some toxic chemicals (e.g., chlorine, methyl mercaptan, hydrogen sulfide
and dimethyl sulfide) are generated [178]. This is not environmentally friendly in large-scale production. To address these problems, Li
et al. reported a lignin-retaining strategy using a bleaching solution (Na2SO3/NaOH/H2O2), showing that>80 % of the lignin content
was retained [151]. Thus, the cell wall of wood does not contain substantial micro- and nanoscale pores (Fig. 2d), which results in a
better-preserved wood structure and favorable mechanical properties under wet conditions. Subsequently, Xia et al. explored an
improved lignin-modification method that consumed less chemicals and energy than the lignin-removal method [124,179]. This rapid
lignin-modification technique was developed by combining H2O2 brushing and photocatalysis (solar or ultraviolet (UV)) to remove
chromophores rather than immersing NW in the bleaching solution. As immersion treatment is not needed, much larger NW (400 ×
110 × 1 mm3 or even up to ~ 1 m in length) can be used to fabricate a strong and robust BWS. This would allow for the potential
Fig. 4. (a) Optical transmittance of TW with different thicknesses. Reproduced with permission [88]. Copyright 2016, American Chemical Society.
(b) Optical transmittance of TWF with different thicknesses. Reproduced with permission [138]. Copyright 2020, American Chemical Society. (c)
Images of the transverse-cut (left) and longitudinal-cut (right) TW and their scattered light spot, respectively. Reproduced with permission [89].
Copyright 2016, Wiley-VCH. (d) Optical transmittance of acetylated and non-acetylated TW. Reproduced with permission [130]. Copyright 2018,
Royal Society of Chemistry. (e) Optical transmittance of TW without or with esterification. Reproduced with permission [182]. Copyright 2020,
Royal Society of Chemistry. (f) Optical transmittance and haze of low/high haze TW. Reproduced with permission [184]. Copyright 2020, American
Chemical Society.
8
scalable manufacturing of larger-scale sustainable wood-based functional materials.

Eliminating light scattering of wood is the second step in fabricating TWMs (Fig. 2a), which can be achieved through two main
approaches: i) the polymer impregnation (backfilling) method and ii) the densification method. For the polymer impregnation method,
the polymers with a refractive index matched with that of the wood cell wall are infiltrated into the BWS under vacuum to obtain TW.
TW was first reported by Fink (in 1992) in a methodology study [154]. Inspired by the transparent crab shell reported by Yano et al.
[87], Berglund’s group developed TW with tunable optical properties and high tensile strength, which was obtained by impregnating
the lumen and cell walls of a balsa BWS with refractive-index-matched polymethyl methacrylate (PMMA, n≈1.49) [88]. At the same
time, Hu’s group backfilled epoxy resin (n≈1.50) into a basswood BWS, resulting in a highly anisotropic and highly transparent wood
composite [89]. Because of the excellent optical transparency (~85 %), haze (~95 %), light-guiding effect, thermal insulation (thermal
conductivity = 0.32 W m− 1 K− 1 along the longitudinal direction) and impact absorption capability, the obtained TW exhibited great
promise as an energy-efficient construction material [61]. Apart from PMMA and epoxy resin, other refractive-index-matched poly
mers [88,180–183], including poly (vinyl alcohol) (PVA, n≈1.53) [153], polyvinylpyrrolidone (PVP, n≈1.53) [125], polyimide
(precursor, n≈1.45) [137], thiol-ene thermosets (n≈1.56) [184], vitrimers [142,185], poly (limonene acrylate) (PLIMA, n≈1.52)
[143]and melamine formaldehyde (MF, n≈1.50) [186], are also suitable alternatives to infiltrate into BWSs for the preparation of TW.
In some cases, the shrinkage of polymers during the polymerization/curing process inevitably causes cracks or defects along the
interface between infiltrated polymers and BWSs, which has an adverse influence on the optical and mechanical performances of TW
[130]. This could be improved by selecting a thiol-ene thermoset with low shrinkage strains as the backfilling polymer to reduce the
interfacial air gaps [184]. Surface modification (e.g., esterification) of BWSs is also used to enhance the interfacial compatibility
between impregnated polymers and BWSs, resulting in improved transparency [130,143,182,187].
Densification is another strategy that converts BWSs into TWMs with or without external forces to obtain TWFs, which is vital to
achieve TWMs with interfacial defects free and high cellulose volume fractions (80 ~ 90 %) [115,138,188–189]. For example, an
anisotropic TWF was prepared with extensive lignin and hemicellulose removal prior to densification and dehydration processes at
room temperature [138–139]. Water molecule-induced hydrogen bonding (microfibrils and cell walls) is driven with the assistance of
compression [190]. The wood cell walls were condensed and collapsed to form a stacked layered structure (Fig. 2a). Another TWF was
produced by self-densifying 2,2,6,6-tetramethylpiperidinyl-1-oxyl (TEMPO)-oxidized mesoporous wood under ambient conditions
without mechanical pressing or heating [191]. Carboxyl groups were introduced to the TEMPO-oxidized cellulose microfibrils within
the cell walls. Once the two sides of the cell walls were in contact, strong hydrogen bonds formed between the abundant carboxyl and
hydroxyl groups on the cellulose microfibrils, leading to complete collapse of the wood cell walls and the formation of a self-densified
TWF. Although this self-densification method is a more facile than routine densification, the introduction of TEMPO treatment is toxic
and thus leads to an environmental issue.
TWMs have been developed for engineering purposes, combining structural and functional performance. The sustainability and
environmental impacts of TWMs are of significance because of the long service time for many applications, such as buildings, elec
tronics and photonics. Berglund’s group intended to improve the fabrication processes and environmental sustainability, for instance,
using UV-light assisted polymerization, selection of bio-based polymers, enhancing compatibility and using green processes
[17,130,143,151,182,184]. On the other hand, Hu’s group and most international researchers emphasize functionalization and the
applications of TWMs. Various functional TWMs can be obtained by modifying the BWS, selecting different backfilling polymers or by
adding functional nanoparticles (Fig. 1) to achieve functionalities including luminescence, magnetic and heat-shielding performance,
strain and gas sensing, conductivity, energy conversion, fire resistance, UV blocking, shape memory, thermal response and man
agement [24,126–128,133–134,138,140,186,189,192–211]. The engineering production cost, scalability and efficiency should be
considered in the future development of TWMs.
3. Structure–property–application
3.1. Structure
Wood has a complex hierarchical structure, from the meter-scale trunk down to nanoscale elementary fibrils and molecular-scale
cellulose chains (Fig. 3a) [212]. Both softwood and hardwood contain different types of cells (for example, vessels and fibers in
hardwood, and tracheids in softwood). The lumens within the cells play an important role in the transportation of water/nutrients in
wood tissue. Cell walls in wood tissue consist of multiple layers, including cell corner middle lamella, middle lamella, primary wall (P),
outer layer (S1), middle layer (S2) and inner layer (S3) of the secondary wall [213]. There are three main components (lignin,
hemicelluloses, and cellulose) and other extractives in the rigid cell walls of wood. The cellulose fibrils are oriented as a skeleton in the
cell wall, embedding in the hemicellulose and lignin matrix [12,214]. At the nanoscale, the strong and stiff cellulose fibril bundles (15
~ 50 nm wide) are constructed from cellulose elementary fibrils (3 ~ 5 nm wide), which are aligned almost parallel along the long
fiberaxis in the S2 layer with small microfibril angles [7]. Various hypotheses have been proposed regarding cellulose biosynthesis in
microfibrils, and it is widely accepted that elementary cellulose fibrils contain a crystalline region where individual cellulose chains are
assembled in an orderly arrangement by intrachain/interchain hydrogen bonding and an amorphous region with a less regular dis
tribution [213]. At the molecular scale, the linear cellulose chains consist of repeating units of D-glucose connected to each other with a
1,4-β-glycosidic linkage (Fig. 3a). Taking advantage of the hierarchical wood structure, porosity and cell wall assembly, novel func
tional wood-based materials can be designed, for example, TW and TWFs.
TW and TWFs have a unique anisotropic structure with highly aligned cellulose microfibrils (Fig. 3b and c). Polymers are suc
cessfully impregnated into the voids and cell walls of the BWS (Fig. 3b center) [143,216–217]. The cellulose microfibrils maintain the
9
(caption on next page)
10
Fig. 5. (a) Stress–strain curves for TW with different cellulose volume fraction, delignified wood and PMMA. Reproduced with permission [88].
Copyright 2016, American Chemical Society. (b) Stress–strain curves of TWF and other materials. (c) The specific Young’s modulus and specific
strength of TWF and other materials. (b-c) Reproduced with permission [138]. Copyright 2020, American Chemical Society. (d) Stress–strain curves
of the anisotropic films with distinct wood cutting angles of 0◦ , 22.5◦ and 45◦ . Reproduced with permission [115]. Copyright 2017, Wiley-VCH. (e)
Stress–strain curves for NW and TW along and perpendicular to the wood channel direction. Reproduced with permission [89]. Copyright 2016,
Wiley-VCH. (f) Stress–strain curves for the transparent plywood. Reproduced with permission [129]. Copyright 2018, Elsevier. (g) Interactions
between BWS and LIMA (left) and stress–strain curves (right) of TW with and without SA modification. Reproduced with permission [143].
Copyright 2021, Wiley-VCH.
original orientation and are densely packed with each other (Fig. 3b right). Similarly, TWFs present a highly aligned cellulose
microfibril structure without polymer impregnation (Fig. 3c right). The densified cell walls show a mortar-and-brick structure at the
cross-section of the TWF (Fig. 3c center). As they retain the anisotropic structure of the BWS, TW and TWFs possess a range of
anisotropic properties, such as mechanical properties, optical performance and thermal conductivity [122].
3.2. Property
The optical, mechanical and thermal properties of TWMs are significantly impacted by several factors at the micro/nano and
molecular scales, such as the cellulose volume fraction, cellulose microfibril orientation and chemical interactions at the cell wall
interfaces. In addition, these properties are also affected by the thickness, porosity and anisotropic structure of TWMs. The experi
mental results are referenced from the literature, as presented in Table 1.
3.2.1. Optical properties

In general, the optical properties of TWMs are characterized by measuring transmittance and haze. Haze can be calculated by the
ratio between the intensity of diffused light and the intensity of total transmitted light [57]. TW has a wide range of tunable trans
mittance (10 ~ 93 %) and adjustable haze (10 ~ 98 %) values, depending on several factors (Table 1), such as wood species, thickness,
cellulose volume fraction and microstructure, which have been summarized in previous reviews [57–58,148]. However, the optical
properties of TWFs have not yet been overviewed. Herein, the effects of wood thickness, anisotropy, lamination and interfacial design
on the optical properties of TW and TWFs (TWMs) are highlighted in this section.
Thickness is one of the main factors governing the optical properties of TWMs. The optical transmittance of TW decreases with
increasing thickness, whereas haze increases [88]. Taking TW (balsa wood) as an example, when the thickness rose from 0.7 mm to 3.7
mm, the transmittance declined from 90 % to 40 %, while the haze increased from 48 % to 80 % (Fig. 4a) [88]. A similar trend was
reported for TW made from beech wood or birch wood [134,218]. This is ascribed to the prolonged light propagation pathway and the
increased interface quantity of polymer/wood, resulting in light attenuation and scattering within TW, respectively. The quantitative
relationship between the total transmittance (Ttotal ) and thickness of TWMs can be expressed by the anisotropic photon diffusion
equation (Equation (1)), showing that Ttotal decays exponentially with increasing TWM thickness [225]. Similarly, the TWF trans
mittance decreases accordingly with the increasing thickness (Fig. 4b). For example, the transmittance of TWFs was reduced from ~
65 % to ~ 60 % when the thickness was increased from 140 µm to 200 µm [138]. This may be explained by the fact that more air-filled
pores are present at increased thickness, resulting in more light scattering in the TWF.
Ttotal = exp( − ad) (1)
where the constant a is the attenuation coefficient and d is the TWM thickness.
The anisotropic structure of TWMs is expected to result in anisotropic properties in the longitudinal and transverse directions of
TWMs. The light scattering pattern is isotropic for TW in the transverse direction (R-wood), whereas light scattering in TW along the
longitudinal direction (L-wood) is highly anisotropic (Fig. 4c). Interestingly, R-wood showed a higher transmittance (90 %) and haze
(~96 %) than L-wood (80 % transmittance and 90 % haze) due to light following the vertically aligned channels of R-wood with high
propagation scattering [89,226–227]. Similar anisotropic light scattering behavior was observed for TWFs [138,191]. Light propa
gation was guided along the wood channel direction, resulting in an anisotropic scattering pattern. The wave-guiding property also
leads to an ellipse-shaped scattering pattern with diverse intensities in the × and y directions.
Lamination is an ingenious way of adjusting the optical properties of TWMs from anisotropic to isotropic. Isotropic TWMs can be
achieved by lamination of several layers with cross-ply or quasi-isotropic structures [129,228–229]. Fu et al. investigated transparent
plywood stacked five-layer structures with different fiber orientations. Instead of the squeezed parallelogram-like scattering pattern of
single-ply TW, an almost circularly scattered pattern was projected for the quasi-isotropic transparent plywood with approximately 75
% transmittance and 80 % haze. The light was confined by the laminated fiber in the transparent plywood structure, leading to
isotropic light scattering performance [129]. Similarly, the lamination strategy can also be used to tune the optical performance of
TWFs. For example, anisotropic TWFs can be assembled into a cross-laminated TWF with a double-layer structure and isotropic optical
properties [115]. In another study, isotropic light scattering and uniform illumination of TWFs was achieved by adding CdSe/ZnS
quantum dots [139]. CdSe/ZnS quantum dots with a core–shell structure can be stimulated by UV light to achieve a quantum yield of
up to 35 %. A ZnS shell layer encapsulating a core layer (CdSe) can passivate surface traps, increasing the nonradiative de-excitation
sites for photon-generated charges. The photoluminescence from the quantum dot core layers diffuse new light through the ZnS atomic
crystalline, which can be uniformly spread over the entire surface of the TWF (approximately 70 % transmittance and 81 % haze)
[139].
11
Interfacial design of cell walls/polymers is an appealing strategy that allows the optical performance of TWMs to be tailored. To
date, esterification strategies have been reported for the chemical functionalization of cellulose microfibrils to design interfaces be
tween cell walls and impregnated polymers [130,143,182,184,187,191,230]. The formation of interfacial gaps usually occurs between
the polymers and the inner cell wall due to different shrinkage ratio and poor interface compatibility [145]. The former can be solved
by selecting polymers with smaller shrinkage ratio, such as thiol-ene thermosets [184]. The latter may be addressed by inducing acetyl
groups on the cellulose microfibrils, which can improve the interfacial compatibility between the acylated BWS and the hydrophobic
polymers (e.g., PMMA). For example, acetyl groups were esterified onto cellulose microfibrils using acetate anhydride, resulting in
improved interfacial compatibility [130]. Compared to the nonacetylated TW, acetylated TW with improved interfacial compatibility
led to an increase in transmittance from 83 % to 92 % (Fig. 4d), while the haze decreased from 70 % to 50 % [130]. Another ester
ification strategy has also been used to modify a BWS to improve interfacial compatibility with impregnated polymers [143,182]. For
example, the chemical modification of a BWS was carried out with renewable cyclic anhydrides, including succinic anhydride (SA),
itaconic anhydride (IA) and maleic anhydride (MA) (Fig. 4e) [182]. The surface modification of the BWS by ring-opening esterification
of anhydrides produces new active sites (e.g., mono- and di-substituted alkenes and terminal carboxylic acid groups), enabling further
interaction with impregnated polymers. Taking the SA-modified BWS as an example, after impregnating PMMA polymer, TW-SA
showed 19 % higher transmittance value and 14 % lower haze value, respectively, than those of unmodified TW due to the
improved interfacial compatibility (Fig. 4e). In a similar report, a fully bio-based TW-esterified material was prepared by impregnation
of a refractive index-matched poly(limonene acrylate) (PLIMA) polymer into an SA-modified BWS with improved interface adhesion,
resulting in 10 % higher optical transmittance and 14 % lower haze than those of unmodified TW [143].
3.2.2. Mechanical properties

The mechanical properties of TW strongly depend on the cellulose volume fraction, wood species, microstructure and wood
densities (Table 1). These have been reviewed by Li et al. but without discussion of TWFs [57–58]. To improve the mechanical
properties of TWMs, both structural manipulation (such as densification and lamination) and chemical modification have been
applied, and these practices are discussed in this section.
Densification of BWSs provides a straightforward strategy to adjust the mechanical properties of TWMs. Cellulose volume fractions
can be controlled by compressing the BWS before the fabrication of TW. With the increase in compression, the cellulose volume
fraction increases, leading to the enhanced tensile strength and modulus of TW. This densification approach was reported by Li et al.,
resulting in an increased Young’s modulus and tensile strength of TW from ~ 2.05 GPa and ~ 38 MPa to ~ 3.59 GPa and ~ 90.1 MPa,
respectively, as the cellulose volume fraction increased from 5 to 19 vol% (Fig. 5a) [88]. This might be related to the synergistic
enhancing effect between the hierarchically/longitudinally oriented cellulose microfibrils and PMMA polymer matrix. In addition, the
Fig. 6. (a) Infrared images of the NaClO-delignified TW (left) and NaClO2-delignified TW (right) indicating the temperature distribution. Repro
duced with permission [66]. Copyright 2019, American Chemical Society. (b) Thermal conductivities of TW and conventional glass. (c) Infrared
image of the anisotropic heat transfer process in the TW. (d) Infrared images of TW with thermal energy distribution in the axial and radial di
rections. Reproduced with permission [136]. Copyright 2020, Springer Nature. (e) The thermal conductivity of axial and radial TW heat directions
at different temperature. (b, c, e) Reproduced with permission [67]. Copyright 2019, Wiley-VCH.
12
densification of BWSs can not only increase the density of the cellulosic reinforcements but also generate more hydrogen bonds be
tween cellulose microfibrils of the densified wood cells, resulting in an enhanced mechanical strength [88,222]. A pure TWF was
designed by a fully densified BWS with highly aligned cellulose and a much higher hydrogen bonding density, which had 3-fold
Young’s modulus (50 GPa) and tensile strength (470 MPa) compared to isotropic cellulose nanopaper (Young’s modulus of 15 GPa
and tensile strength of 150 MPa) (Fig. 5b) [138]. Its specific strength was greater than that of most natural fibers, fossil-based plastics
and polymers (Fig. 5c). This positions the material at a prominent location in the Ashby chart, with excellent mechanical performance
but lightweight characteristics (Fig. 5c) [138]. A self-densified film was also reported, yielding a high Young’s modulus (51.1 GPa) and
tensile strength (449.1 MPa) [191]. The mechanical performances of TWFs can be tuned by adjusting the cutting angle (the angle
between the fiber direction and cutting direction) from NW. The lower cutting angle (ϴ = 0◦ ) achieved a TWF with higher cellulose
alignment and anisotropy resulting in a high tensile strength (350 MPa), whereas a higher cutting angle (ϴ = 45◦ ) produced a TWF
with a reduced strength (190 MPa) due to decreased cellulose alignment in the loading direction (Fig. 5d) [115]. The densification
strategy can prevent the density variability caused by different wood species, providing a convenient and feasible strategy for regu
lating the mechanical properties of TWMs.
Lamination of transparent veneers was found to play a prominent role in overcoming anisotropy and producing an isotropic TWM.
The intrinsic anisotropic structure of TWMs leads to different mechanical properties in the longitudinal and transverse directions
(Fig. 5e). The tensile strength (45.4 MPa) of L-wood is two times as high as that of transverse TW (23.4 MPa, R-wood) [89]. Most
currently reported TWMs are either thin or anisotropic (Table 1) [67,129,139,220]. However, transparent plywood, with a cross-
laminated or quasi-isotropic structure, can be relevant in various emerging applications where isotropic mechanical properties are
crucial. Plies of transparent balsa veneers were laminated by controlling the wood fiber direction and thickness (>3.5 mm), resulting in
an isotropic TWM. The ultimate strength of transparent plywood increased from 15 MPa to 45 MPa under transverse loading (Fig. 5f)
[129]. As a consequence, the transparent plywood fabricated by the laminating method demonstrated isotropic mechanical properties
in both the longitudinal and transverse directions [220]. By applying this lamination technique, the mechanical properties of the TWM
are controllable and predictable based on the mechanical modeling of laminate plate theory.
Chemical modification can functionalize the surface of wood fibers, which can enhance interfacial bonding, thus improving the
mechanical performance of TWMs. For instance, Montanari et al. reported a fully bio-based TW prepared by the diffusion of limonene
acrylate (LIMA) monomer into the SA esterified cell wall [143]. After polymerization, the LIMA polymers were covalently linked to the
functionalized BWS, resulting in a fully bio-based TW with a high mechanical strength of 174 MPa and Young’s modulus of 17 GPa
(Fig. 5g). The chemical modification route is applicable to a variety of wood species, allowing tunable mechanical performance of the
TWM. Other chemical modification methods, e.g., acetylation and TEMPO-oxidation, can potentially be applied to tailor the wood
fiber/polymer interfacial adhesion, achieving mechanically robust TWMs (Table 1) [130,191].
3.2.3. Thermal properties

With the demand for energy-saving building materials in the building sector, thermal insulation properties become essential for
controlling heat exchange. The thermal conductivity is determined by the different wood compositions (the total volume fraction of the
BWS in TW) and anisotropic microstructure of TW. TW with ideal thermal insulation exhibits great potential for application as a
transparent and energy-efficient building material (Table 1).
Fig. 7. The actual performance comparison of between (a) glass and (b) TW. (a) Low thermal energy efficient image: Reproduced with permission
[15]. Copyright 2018, Wiley-VCH. Glaring and highly brittle images: Reproduced with permission [61]. Copyright 2016, Wiley-VCH. (b) Repro
duced with permission [61]. Copyright 2016, Wiley-VCH.
13
Fig. 8. Diagram of TW applied to transparent and smart buildings. (a) Letter A and yin-yang patterned TW. Reproduced with permission [124].
Copyright 2021, American Association for the Advancement of Science. (b) The photo of aesthetic TW, and its demonstration as an aesthetic rooftop
material. Reproduced with permission [136]. Copyright 2020, Springer Nature. (c) Schematic to demonstrate the TW used as clear wood windows,
and its digital images. Reproduced with permission [66]. Copyright 2019, American Chemical Society. (d) Temperature changes in model houses
with glass (right) and CsxWO3/TW (left) as windows after 10 min of simulated solar radiation. Reproduced with permission [128]. Copyright 2017,
Royal Society of Chemistry. (e) Temperature changes inside the box with infrared light irradiation. Insets are images showing the color changes of
ATO/TW with UV irradiation. Reproduced with permission [150]. Copyright 2019, Elsevier. (f) Schematic representation of thermal energy storage
and tunable transmittance by varying the temperature. Reproduced with permission [134]. Copyright 2019, American Chemical Society. (g) For
mation mechanism illustration, SEM and EDS images of cationic silica-TW. Reproduced with permission [202]. Copyright 2022, Wiley-VCH. (h)
Photograph to illustrate the self-extinguishing property. Reproduced with permission [137]. Copyright 2022, Elsevier. (i) Illustration of a low heat
release value. Reproduced with permission [186]. Copyright 2022, Elsevier.
Thermal conductivity is affected by the volume fraction of the BWS in TW. The impact of different delignification processes (NaClO-
delignified vs NaClO2-delignified) on the thermal conductivity of TW was investigated by Jia et al. [66] NaClO2-delignified TW
possessed a slightly lower thermal conductivity (0.24 W m− 1 K− 1) than NaClO-delignified TW (0.35 W m− 1 K− 1) because NaClO2-
delignified TW had a significantly higher wood component volume (18.4 vol%) than NaClO-delignified TW (2.9 vol%) (Fig. 6a) [66].
The TW had a much lower thermal conductivity of 0.35 W m− 1 K− 1 along the fiber direction, which is only one-third of the thermal
conductivity of glass (~1 W m− 1 K− 1) (Fig. 6b). This is attributed to the complex organization of the hierarchical cell wall structure
(Fig. 3a), which can lead to high resistance to phonon transportation within the cell walls (mainly composed of cellulose and hemi
cellulose) due to the increased phonon scattering at the numerous interfaces [61]. Therefore, TW with the desired thermal conductivity
can be achieved by controlling the wood composition and microstructure during the delignification process.
Thermal properties are also dominated by the anisotropic microstructure of TW. The thermal energy tends to transfer along TW
with an ellipse shaped distribution under heat radiation (Fig. 6c) [67]. This can be explained by the fact that heat preferentially
propagates along the well-preserved wood cell walls, which yields less phonon scattering along the wood channel direction than in the
vertical direction. Moreover, the irradiated phonons are blocked or confined to travel through the nanoscale pores in the cell walls
[61], resulting in a lower thermal conductivity in the radial direction than in the axial direction (Fig. 6d) [136]. When the heat source
is in the temperature range from 20 ◦ C to 60 ◦ C (Fig. 6e), TW shows a low thermal conductivity (~0.19 W m− 1 K− 1) in the radial
direction and a higher thermal conductivity (~0.4 W m− 1 K− 1) in the axial direction. However, both values are still much lower than
those of traditional glass [67]. In this context, structural manipulation by tuning compositions and/or pore structures provides a
possibility to govern the thermal properties of TWMs. However, the thermal properties of TWFs have not been investigated.
14
3.3. Application
3.3.1. Transparent and smart building materials: TWM as an alternative to glass

Developing energy-efficient building technologies is expected reduce residential energy consumption (such as in cooling, heating,
lighting and electrical usage),targeting 50 % or more reduction [231]. Energy-efficient buildings require less energy consumption
while creating a comfortable environment for their occupants. In addition, energy-efficient buildings with low-cost illumination and
thermal insulation can reduce the carbon footprint while contributing to reducing global warming, and providing financial savings. To
this end, the actual performance and economic viability of energy-efficient buildings have gained great attention.
Glass is one of the most common high-transparency and low- haze building materials. However, it has some limitations when used
in buildings (Fig. 7a) [15,61]. (1) Glass has very low energy efficiency due to its high thermal conductivity (~1.0 W m− 1 K− 1), allowing
for the rapid exchange of heat energy between the outdoors and indoors. (2) Reflection effects and discomforting glare from glass may
occur during the daytime, impacting working efficiency and emotional well-being and sometimes leading to traffic accidents due to
‘sun strike’ [61]. (3) Glass has potential safety issues as it can be broken and shatter immediately with a sudden mechanical shock,
long-term creep deformation or earthquakes (Fig. 7a) [15]. (4) The production of glass results in 25 thousand tons of carbon dioxide
every year, contributing to climate change and global warming [15].
Interestingly, TWMs are considered promising candidates as energy-efficient building materials in the substitution of glass, mainly
for the following reasons (Fig. 7b). (1) Excellent thermal properties: TW possesses a lower thermal conductivity (0.19 ~ 0.39 W m− 1
K− 1) than glass, which can effectively reduce energy loss [67]. (2) Well-being in indoor environments: TW can create a comfortable
indoor lighting environment in the daytime. (3) Better security: TW has an improved mechanical toughness (0.56 ~ 6.1 MJ m− 3, glass
= 0.1 MJ m− 3), preventing sudden shattering [66,89,130]. (4) Environmentally friendly: TWMs are relatively ecofriendly because the
BWS derives from biodegradable, renewable and sustainable NW. More promisingly, impregnated resins are moving toward more
environmentally friendly polymers, such as biomass-derived PLIMA and biodegradable PVA. These merits are driving research and
Fig. 9. (a) Schematic of display photochromic TW windows on a building with solar irradiation. Reproduced with permission [132]. Copyright
2019, Royal Society of Chemistry. (b) Images of the electrochromic TW device. Reproduced with permission [63]. Copyright 2018, Wiley-VCH. (c)
Photograph of a luminescent TW stool. Reproduced with permission [151]. Copyright 2017, Wiley-VCH. (d) Illustration of a uniform illumination
using a luminescent TWF as a lighting panel/cover when exposed to a UV light source. Reproduced with permission [139]. Copyright 2020,
American Chemical Society. (e) Optical images and UV spectrum of reconstructed wood. (f) Schematic showing the photothermal conversion device.
(e-f) Reproduced with permission [224]. Copyright 2022, Elsevier.
15
development of TWMs as energy-efficient building materials for various applications (Fig. 8).
TW is considered a promising transparent building material for aesthetic and optical design. Xia et al. demonstrated patternable
TW, showing various patterns, such as the letter A and a yin-yang symbol (Fig. 8a) [124]. By applying a solar-assisted chemical (H2O2)
brushing method, the desired patterns of NW turned white. After infiltrating epoxy into the white BWS, the patternable TW can be
precisely designed. In addition, aesthetic TW with natural annual ring features can be fabricated owing to the gradient distribution of
lignin between late and early NW (Fig. 8b). Further aesthetic patterns were achieved by laminating multiple layers of TW. These
aesthetic TW materials were demonstrated as a patterned ceiling in a museum or gallery, where natural light and aesthetic patterns can
be uniformly projected to the indoors (Fig. 8b), which may not happen from glass [136]. Optically designed TW with tunable haze can
be prepared by different delignification processes (NaClO vs NaClO2), as well as tailored interfacial adhesion [66–67,143,184]. Clear
TW with 10 % haze was made by a NaClO delignification process, enabling an appealing substitution of common glass in an energy-
efficient window (Fig. 8c). Translucent TW with approximately 80 % haze can be obtained by the NaClO2 delignification process,
allowing for lightening but with the protection of personal privacy [61,66]. These optical and aesthetic design options with TW
materials provide routes for replacing traditional glass in some engineering applications.
The structural design offers opportunities to achieve large TW as alternatives to glass, such as windows and buildings. TW has been
proposed as a building material that combines structural and functional performances [61]. As a proof-of-concept, a house frame was
demonstrated using a TW roof with more uniform illumination and better thermal insulation performance than a glass rooftop [61]. To
meet the requirements of building applications, TW materials with larger dimensions and higher thicknesses need to be developed. Fu
et al. reported load-bearing and luminescent TW (thickness = 3.5 mm) based on the lamination technique. Transparent plywood can be
designed by cross-stacking layers with an isotropic structure. This improved the mechanical properties in the weakest direction by
controlling fiber orientations and resulted in TW with tunable light scattering behavior [129]. A green steam-modification (H2O2/HAc
steam) method was developed to uniformly modify lignin in bulk wood, resulting in translucent wood with 2 ~ 5 cm thickness that can
be used as a building material [232]. More recently, Xia et al. proposed a scalable technique combining H2O2 lignin modification and
photocatalytic oxidation processes to create large TW (400 × 110 × 1 mm3). This simple, fast and scalable fabrication of TW com
posites shows great potential for TW to be used as a next-generation building material [124,136]. As a demonstration, these large TW
materials have been showcased as a window or model building (Fig. 8c) that can efficiently harvest sunlight for uniform indoor
illumination, so they can potentially replace conventional glass. Near-infrared light (wavelength λ = 800 ~ 2500 nm)-absorbing
nanoparticles and phase-changed polymers have been encapsulated in TW, resulting in heat-shielding or thermal energy storage
composites that have potential applications in energy-efficient buildings. For example, CsxWO3 or antimony-doped tin oxide (ATO)
nanoparticles were embedded in TW composites, which were demonstrated for thermal-shielding buildings/windows (Fig. 8d)
[128,150]. Due to the near-infrared light being absorbed by the nanoparticles, a much smaller temperature increase was achieved from
these functional TWs compared to that of normal TW and glass [67,128,150]. Functional TW with ATO also demonstrated improved
antiaging performance and prolonged service life (Fig. 8e) [150]. Thermochromic heat-shielding is another important application for
TW materials. Tungsten-doped vanadium dioxide nanoparticles can reflect near-infrared light and reduce the phase transition tem
perature to room temperature, allowing infrared radiation to be transmitted below room temperature and mostly reflected above room
temperature [205]. In another study, TW for thermal energy storage was designed by adding phase-change materials into a BWS
[134,233]. For example, a polyethylene glycol/PMMA polymer blend was impregnated into a porous BWS, enabling TW to store/
release thermal energy [234–235]. The thermal energy storage/release ability of TW can be adjusted by heating above the melting
temperature or cooling until the crystallization temperature of the polyethylene glycol polymers is reached [134], which cannot be
Fig. 10. Characteristic comparison of plastic and TWF. (a) Reproduced with permission [15]. Copyright 2018, Wiley-VCH. (b) Reproduced with
permission [223]. Copyright 2018, American Chemical Society.
16
achieved with glass (Fig. 8f).

The impregnation of flame retardants into a BWS can improve the fire safety of TWMs in the applications of building materials. This
can be achieved by the incorporation of inorganic particles, phosphate- or nitrate-based retardants [137,186,199–200,202,236], such
as MXene nanosheets and silica nanoparticles, polyimide, MFs and phosphate ester-polyethylene glycol (PEAG) polymers. The wood
cell walls were enriched with carboxyl groups, enabling effective permeation of cationic silica nanoparticles and a uniform distribution
of inorganic nanoparticles inside the cell walls (Fig. 8g). An inorganic surface layer formed in the functional TWM, resulting in a
favorable fire retardancy, with limited oxygen permeability and little degradation of volatile gases [199,202]. A phosphate- or nitrate-
based polymer with a refractive index similar to that of the BWS, was impregnated and processed into fire-retardant TW. Due to the
carbonization of polyimide/MF or PEAG chains and the formation of a protective char layer in the combustion test, the resultant TW
exhibited an outstanding self-extinguishing property (Fig. 8h), low heat release (Fig. 8i) and flame retardancy [137,186,200]. These
TW materials also showed higher ignition and lower total smoke release values than NW, suggesting their great potential as a novel
type of fire-retardant transparent composite in building material applications.
Tunable UV-blocking property enables TWM as a smart window, protecting human skin, furniture and interior displays from hazard
and damage. Retaining lignin, adding organic absorber (e. g., 1,3,3-Trimethylindolino-6′ -nitrobenzopyrylospira., 2-(2H-Benzotriazol-
2-yl)-4, 6-di-tert-pentylphenol, CNF, chitosan, lignin) or inorganic UV absorber (e. g., ATO, γ–Fe2O3@YVO4:Eu3+, SrAl2O4:Eu2+,Dy3+)
can realize the UV protective performance of TWMs [127,150,193,209,224,236–240]. Organic UV absorbers can capture the UV
energy and convert it to other forms of energy, which is attributed to the chromophore and auxiliary groups connected with aromatic
groups, such as C– – N, N–N, –NH2, –OH, -SO3H and –COOH. For example, by spatially selective delignification of wood cells or the
addition of organic UV absorbers, TWMs displayed a low transmittance in the UVA (320 ~ 400 nm), UVB (275 ~ 320 nm) and UVC
(200 ~ 275 nm) regions [238]. Different from the light energy conversion, inorganic UV absorbers can connect with wood microfibrils,
followed by increasing the reflection and scattering of UV light on their surfaces, preventing UV rays from passing through TWMs to
achieve the UV protection effect. After embedding the inorganic UV absorbers, the UPF values (a parameter to estimate UV blocking) of
TWMs were 15 ~ 21 times than that of blank sample, indicating an excellent UV protection ability of TWMs [209,237].
Functionalized TWMs allow for smart applications, for instance, as photochromic, electrochromic, luminescent, and photothermal
conversion windows [63,126,132,140,146,151,224,237,241]. A photochromic smart window was prepared by infiltrating a BWS with
a photochromic material/MMA blend, showing photoswitchability between purple and transparency with illumination (Fig. 9a). Light
transmittance was controllable by the photochromic material-doped TW due to the reversible chemical structure of spiropyran/
merocyanie [132]. Inspired by this concept, Samanta et al. reported a double-stimulus-responsive chromic TW where the optical
performance was reversibly tailored by changing the temperature and UV radiation [206]. A smart electrochromic TW device was
assembled, and the transparent conducting electrode was prepared by coating poly(3,4-ethylenedioxythiophene):poly(styrene sul
fonate) on TW. The color could be switched when 0.8 or − 0.5 V was applied to the electrochromic TW device (Fig. 9b) [63]. In a
luminescent lighting application, CdSe/ZnS quantum dots were incorporated into a TWM, resulting in a luminescent and light scat
tering material that could be applied in lighting panels as a replacement for glass (Fig. 9c-d) [126,139,151]. The combination of
TEMPO-oxidized wood films and lignin enables excellent water resistance and UV-shielding performance (Fig. 9e) [224]. Due to the
high absorption in the near-infrared spectral region and low reflectance in the solar spectrum, this TWM displayed great potential in
photothermal conversion devices (Fig. 9f). Based on the above descriptions, these functional TWMs may have potential in applications
where glass is commonly used, such as windows, lighting covers/panels and energy-efficient buildings.
3.3.2. Optoelectronic devices: TWM as an alternative to plastics

There is a growing demand for optoelectronic devices, such as laptops, smart phones, televisions, portable electronics and displays
[242–249]. However, the substrates of these devices are typically made of nonbiodegradable and/or nonrenewable glass or plastics. In
particular, most plastics used for optoelectronic devices are fossil-based. They are frequently upgraded and discarded due to the rapid
development of advanced technologies, which have led to serious environmental contamination, for example, land, seabed and air
pollution (Fig. 10a) [15,250]. Moreover, these electronic wastes usually contain hazardous inks or semiconductors (e.g., gallium
arsenide or heavy metals) that can release toxic substances, causing major environmental concerns and human health problems [96].
This has motivated a search for excellent alternative substrates with high transparency, flexibility, printability and more environ
mentally friendly features (Fig. 10b) [223,251]. The recent development of TWMs drives the production of fully bio-based and eco-
friendly materials, which can fulfill these requirements and have demonstrated great potential to gradually replace all-plastic-
based substrates in optoelectronic devices [89,125,223].
Due to their high transparency and low thermal expansion coefficient, TWMs have recently been explored as substrates for
replacing fossil-based plastics, enabling their application in flexible electronics [252–253]. A flexible TW substrate with high trans
parency (80 % transmittance) was demonstrated by coating silver nanowire (AgNW) ink on a TW substrate using the Meyer method
(Fig. 11a). The as-prepared conductive substrate with a sheet resistance of 11 Ω sq-1 could illuminate a light-emitting diode (LED), even
when being bent [131]. Another study reported spray coating AgNWs on TW, achieving a much lower sheet resistance (3 Ω sq-1) and a
stable conductivity after 500 bending test cycles (Fig. 11b) [133]. By sandwiching a luminescent layer between two conductive
electrodes, a three-layer alternating current electroluminescent (ACEL) device was successfully fabricated with a luminance value of
18.36 cd m− 2 (voltage = 220 V, frequency = 1 kHz). More interestingly, the BWS can effectively limit the volume expansion of the
ACEL devices. Due to the addition of the BWS with a low coefficient of thermal expansion (0.1 × 10-6 K− 1), TW showed a lower
coefficient of thermal expansion (5 × 10-6 K− 1) than polyethylene terephthalate (PET) [(86.37 ± 3.62) × 10-6 K− 1] and epoxy [(76.89
± 3.53) × 10-6 K− 1], providing favorable dimensional stability of the TW substrates in ACEL devices. The flexible ACEL device also
demonstrated good thermal stability and waterproofing properties and could retain good luminescence properties at 100 ◦ C for 30 min,
17
in water for 30 min, or even at 90 ◦ C and 90 % relative humidity for 30 min (Fig. 11c). The values were comparable to those of common
plastics, such as PET, nylon, polyethylene, polyvinyl chloride and epoxy [204]. Interestingly, various patterns can be fabricated,
indicating versatile material design concepts in high temperature-resistant and programmable ACEL devices (Fig. 11c) [204]. Based on
environmental concerns, a full cellulose-based TWF was demonstrated to be a biodegradable transistor. After placing the device in soil
and exposing it to nature for 6 days, the TWF electronic device disappeared from the soil, suggesting fast degradation of the device
[223]. Very recently, an environmentally friendly all-biobased TWM was developed by infiltrating a renewable and biodegradable CNF
or chitosan aqueous suspensions into a BWS. Due to the hydrogen bond interaction between CNF/chitosan and the BWS, a TWM with
high transmittance (80 %), adjustable haze (30 ~ 60 %), good thermal stability (315 ℃) and excellent UV shielding properties was
produced, holding great potential as a substrate for flexible electrodes [240].
TWMs have demonstrated applications in sensors due to their anisotropic structure and excellent flexibility [138,140,203]. For a
strain sensor, Fu et al. proposed the highly efficient utilization of all wood components combining a TWF and lignin-derived
carbonized fiber ink [138]. Through directly printing lignin-derived conducting ink on the TWF substrate, a fully wood-based flex
ible film could be produced as a flexible strain sensor. The TWF electronic circuit showed a more stable electromechanical performance
than PET plastic, as the TWF circuit had less deformation/detachment from the substrate when the circuit was loaded. Moreover, these
circuits could activate LEDs when they were bent and folded, indicating favorable flexibility and conductivity (Fig. 11d left and
middle). The anisotropic structure of TWFs provides further opportunities in this regard. As a proof of concept, a hand-held TWF strain
sensor along the transverse direction (vertical with wood fiber orientation) showed variation in relative resistance with finger
movement (Fig. 11d right). Wang et al. reported novel stretchable and conductive TW by backfilling nontoxic polymerizable deep
eutectic solvents (PDES and acrylic-acid/choline chloride) into the pores of a BWS via in situ photopolymerization. Due to the hydrogen
bonding of PDES and the BWS, the obtained TW exhibited high transparency, stretchability, electrical conductivity and sensing ability
to external stimuli (e.g., strain and touch), which could be applied to monitor human activities and subtle pressures [203]. Based on
this work, Yang et al. further reported flexible TW using the same PDES, and they discovered the temperature sensing properties of the
TW. When the temperature increased or decreased, the conductivity of the flexible TW increased or decreased monotonously. This
favorable temperature-sensing feature makes TW a promising candidate as a temperature sensor [254]. Recently, superflexible TW
fabricated by impregnating biocompatible and flexible poly(ethylene glycol) diacrylate into a BWS was reported, serving as the TW-
based electrode for a pressure sensor after coating AgNWs. By sandwiching two TW-based electrodes and a stimuli-responsive layer
with a pyramidal microstructure, a flexible wood-based e-skin with capacitive and optical dual-response sensitivity was developed,
showing both naked eye- and instrument-readable features. This wood-based e-skin could make an electroluminescent response within
the range of pressures (0 ~ 150 kPa) that humans experience pain and maintain a high sensitivity (>0.15 kPa− 1) [144]. For the
application of TWMs in gas sensors, Liu et al. developed a smart construction material with timely and visible self-detection of
formaldehyde (FA) gas. It was fabricated by encapsulating a gas sensor consisting of a blend of multicolor carbon dots (CDs) and PVA.
The CDs/PVA TW demonstrated the ability to self-detect indoor FA by visual color-responsive ratiometric fluorescence and delayed
room temperature phosphorescence [140].
TWMs have the potential to replace plastic/glass substrates in solar cells or WLEDs because of their high light transmission and
scattering performance [125,135,140,169,255–256]. A light scattering TWM was used as a light management material for a GaAs solar
cell device with an enhanced total conversion efficiency of 14 ~ 18 % (Fig. 11e) [125,255]. This could be ascribed to two reasons: (1)
Light reflection was reduced using the light scattering TWM, resulting in more light propagating through the coating layer to the GaAs
solar cell. (2) The incident light was diffused due to the high haze (~80 %) of the light scattered TWM, extending the photon-traveling
path and improving light trapping performance. Similarly, an assembled TW perovskite solar cell showed a high power conversion
efficiency of 16.8 % and favorable long-term stability [135]. Beyond solar cells, the large light scattering effect also allows TWMs to be
candidates for the encapsulation material of WLEDs [140,169,198,201]. A green WLED TW was prepared by mixing citric acid-derived
multicolor CDs with acrylic acid, followed by incorporation into a BWS [169]. The TW-based encapsulation material, together with a
blue UV-chip, was assembled into a promising WLED device, which displayed excellent color characteristics with a Commission on
Illumination value of (0.33, 0.32) and good luminous stability for 7 days (Fig. 11f). Apart from citric acid-based CDs, lignin-derived
CDs doped with various nitrogen-containing compounds could also be brought into wood cells as trichromatic systems for TW-based
encapsulating materials [140,201]. By infiltrating the multicolor-emission lignin-based CDs and PVA or UV curing resin into a
delignified wood frame, outstanding encapsulation films of WLEDs were achieved and showed uniform white light under a UV lamp
[140,201], as well as resistance to water, acid, alkali and salt, with a stable light-emitting performance [198]. Thus, TWMs demon
strate great potential to replace plastic/glass substrates for clean energy conversion/storage devices.
Based on the discussion in Section 3.2, TWMs benefit from their anisotropic structure, showing tunable optical, mechanical and
thermal properties. As a result, they are regarded as alternatives to glass and plastics in a wide range of applications, including energy-
efficient buildings, smart windows, flexible optoelectronics, sensors, energy conversion and storage devices. Structural design concepts
allow for the manipulation of the microstructure and chemical compositions of BWSs, as well as for laminated and densified structures.
The functional design concepts enable the achievement of additional functionalities, such as conductivity, thermal insulation, thermal
storage, luminescence, photon response and electroresponse. Combining the functional and structural performances of TWMs endows
them with great potential as an engineered replacement for glass and plastics and in other advanced applications (e.g., automobile and
aircraft materials).
4. Process–structure–property–application relationships
TWMs integrate load-bearing properties with photonics functions and light weight. The cellulose microfibril skeleton in the cell
18
wall is a sophisticated reinforcement structure, and chemical/physical treatments can be used to tailor the nanostructured BWS. In
addition, functionalization strategies enable the addition of new functions/properties to TWMs for specific applications. To this end,
fundamentally understanding the process–structure–property–application relationships of TWMs is essential for engineering purposes.
(1) Process–structure relationship: Currently, wood nanotechnologies including various chemical and physical treatments are
applied to tailor the composition and microstructure, resulting in a fully/partly delignified BWS with a wide range of Bru
nauer–Emmett–Teller specific surface areas (1 ~ 260 m2/g, Table 1). The influence of these treatments on the chemical reactions and
components of different wood cell walls (e.g., balsa, pine, poplar, ash, beech and basswood) is not fully understood. For example, the
extraction of the lignin component is complicated in bulk wood. Moreover, uniform delignification of a global wood structure,
particularly in the thickness direction, is always a challenge because of the limitation of chemical penetration into the cell wall. Thus,
efficient and controllable delignification processes are being developed. Furthermore, greener chemical treatment of wood with a high
porosity should be considered for future investigation, as a highly porous material provides many interactive sites for the function
alization step. Low carbon emission processes could be adapted to a continuous roll-to-roll production system with aiming at large-
scale production [138]. Extending these wood nanotechnologies to other natural plants for designing new materials, such as
bamboo, reed and loofah templates, is also of great interest [257–266].
(2) Structure–property relationship: A basic understanding of the impact of the structure–property relationship is crucial for the
material design concept and adding new functionalities to TWMs. There is a lack of knowledge of the underlying structure–property
relationships of nanostructured wood and how to manipulate these specific nanoeffect properties. Wood nanoscience has developed
from multidisciplinary theories, such as the nanoconfinement effect, supermolecular topology, permeability theory and optic physics,
which are applied to answer the scientific questions of TWMs. For example, how do photons, electrons and ions travel/transport within
the nanostructure of TWMs? From a technological point of view, the high performance of TWMs (optical, thermal and mechanical
properties) can be achieved by adapting the volume fraction, thickness, lamination and chemical modification/functionalization of
BWSs. Specifically, by tailoring the wood thickness and volume fraction and applying lamination and interfacial design strategies,
TWMs can achieve suitable optical properties. To achieve the expected mechanical properties of TWMs, structural manipulation by
densification and lamination can be applied, as well as chemical modification. For thermal properties, changing the volume fraction of
the BWS or anisotropic microstructure can be adopted. Moreover, advanced characterization techniques (e.g., computational simu
lation, X-ray synchrotron and micro computed tomography, and ultrahigh transmission electron microscopy), are required for the
development of wood nanoscience and nanotechnologies, and to obtain a fundamental understanding of the physics of TWMs. Further
investigations of the chemical interactions will help us to control their microstructure for tunable properties.
(3) Property–application relationship: Our review emphasizes the mechanical, optical and thermal properties, as well as relative
emerging applications (electronics, photonics, sensors and energy storage devices). Although many chemical modification and
functionalization strategies have been proposed to achieve multifunctional TWMs and have been demonstrated in various applications,
the development of TWMs is in an early stage. TW replies on the impregnation of refractive-index-matched polymers with additional
functions. An appealing strategy is to functionalize the BWS prior to conversion into TWMs, which may realize new opportunities for
making multiple functional TWMs possible. In addition, most applications of TWMs are at the proof-of-concept stage, with a
considerable amount of work required to achieve commercialization and large-scale production. The impact on our society may not be
realized immediately; thus, future research should pay attention to realistic demands and the connections between functionalities and
real applications in our lives.
5. Summary and future outlook
TWMs are an exciting option for next-generation wood-based materials. The top-down method is a powerful strategy to convert
bulk wood into functional and sustainable materials, making a large-scale production possible. Wood nanotechnology has been
developed for engineering the production of TWMs with combined structural and functional performances. This review has over
viewed the state-of-the-art research covering the transparency mechanism, processing methods, structure, property, application and
their relationships.
One may ask the justification behind converting wood into a transparent material by the top-down method, specifically, instead of
the already-matured nanocellulose-based transparent materials prepared via the bottom-up approach. Although the formation of
nanocellulose-based materials provides greater control of the material structure, it requires multiple energy-intensive and time-
consuming steps, starting with nanocellulose deconstruction from the plant cell wall and ending with the reconstruction of new
material structures via bottom-up assembly. Note that the nanocellulose deconstruction process may consume ~ 500 kWh ton-1 to 30
000 kWh ton-1 energy depending on the native or modified state of the cell walls (e.g., fibers), leading to an estimated cost of over $50
~ 100 kg− 1 [267]. Furthermore, the inherent anisotropic hierarchical structure of wood is damaged, which requires the reconstruction
of small building blocks to achieve transparent materials.
The justification for making wood transparent lies in the fact that TWMs incorporate all the advantages of nanocelluloses, such as
their light weight, excellent mechanical and light transmission properties, and high thermal stability, but energy-intensive and time-
consuming deconstruction and reconstruction processes are not needed. The excellent inherent anisotropic characteristics of wood
have led to unique anisotropic optical, mechanical and thermal functionalities. The ease of functionalization of the BWS via chemical/
physical modification and nanoparticle impregnation has led to the fabrication of TWMs with additional features, such as high optical
transmittance, adjustable haze, mechanical flexibility, luminescence, photo- and electrochromic performance, heat and UV resistance,
flame retardancy, and gas sensitivity.
However, there are still some challenges to tackle in TWM research. One of the major challenges, for example, is to produce a
19
Fig. 11. Diagram of TWM applied to flexible optoelectronic devices. (a) Schematic to demonstrate a LED lighted up by a flexible and conductive TW
before and after bending, respectively. Reproduced with permission [131]. Copyright 2018, Royal Society of Chemistry. (b) A flexible and
conductive TW with an excellent conductivity stability even after 500 bending tests. Reproduced with permission [133]. Copyright 2019, American
Chemical Society. (c) Schematic to diagram the ACEL device and its excellent luminescence stability and different illumination modes. Reproduced
with permission [204]. Copyright 2019, American Chemical Society. (d) Photographs of the conductive TWF and its application for strain sensors.
Reproduced with permission [138]. Copyright 2020, American Chemical Society. (e) Application of TW/GaAs solar cell. Reproduced with
permission [125]. Copyright 2016, Elsevier. (f) Luminous stability of the TW/CDs WLEDs in 7 days. Inset is a photograph of a lighting WLED.
Reproduced with permission [169]. Copyright 2018, American Chemical Society.
sufficiently large and thick TWM for commercial implementation. This is partly because the integrity of the BWS with uniform cell wall
penetration is difficult to maintain after delignification treatment. Lignin is known as the gluing material among the fibers. The
removal of lignin essentially makes the BWS delicate to handle for further processing. Although lignin-retaining/modified methods
have already been developed, more investigation is needed to optimize lignin modification or to develop new efficient delignification
methods that would not sacrifice the optical properties and thickness of the TWM.
Another challenge is to obtain optically clear wood with a haze below 10 %. Most of the currently reported TWMs have a haze value
of 40 ~ 80 % depending on their thicknesses. Recently, optically clear wood has been reported to have a high transmittance of 90 %
20
and a low haze of 10 %, but the cellulose fraction was only 2.54 vol%. This led to a negligible improvement in the strength properties
compared to those of the constituents. On the other hand, the haze value of a nanocellulose-based transparent material, despite having
similar constituents with a nanocellulose content as high as ~ 70 %, can easily reach below 10 ~ 20 %. The elucidation of the un
derlying reasons for this phenomenon may eventually lead to a strong, highly optically clear wood for next-generation applications.
To date, little attention has been focused on the trade-off of the stability and biodegradability of TWMs through their life cycle, as
well as the production cost. The optical and mechanical properties of TWMs may be slightly impaired when they are exposed to water,
fire or UV irradiation, owing to the biodegradable and hydrophilic characteristics of the wood components. Although there have been
reports on functionalization, such as UV absorption and hydrophobic modification, how to achieve a stable yet biodegradable TWM
with a certain stimulus response is a promising direction for future research. Future research should aim at lowering the production
cost of TWMs with bio-based polymers and environmentally friendly processes, as well as developing new processes suitable for
manipulating TWM structures with controlled micro- and nanostructures.
Overall, wood nanoscience and nanotechnology are new and developing topics in the material science field. A better understanding
of the science (the processes–structures–properties–applications relationships) of TWMs is essential for both academic and industrial
communities to drive their progress. A combination of emerging technologies (e.g., machine learning, artificial intelligence, 3D
printing and big data) will enable commercialization and support our sustainable modern society in the future. This will benefit to the
sustainable development of structural and functional TWMs in the extension of carbon storage and replacement of nondegradable
plastics. It is also crucial to address the fundamental science and physics of TWMs that have inspired and been integrated with other
disciplines, such as wood science, material chemistry and physics. All future challenges aside, derived from the abundant advantages
reported thus far, the global overview of the TWMs in the current review will serve as an indicator and establish new insights for
developing the topic. We foresee that TWMs have an enormous potential to replace glass and fossil-based plastics, expanding their
future application in sustainable smart buildings, optoelectronics, clean energy conversions, sensors, e-skins, soft robotics and other
emerging fields.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to
influence the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgments
S. L. Zhu and S. K. Biswas contributed equally to this work. We acknowledge the National Natural Science Foundation of China
(31901274), Canada Research Chairs Program (231928), 13th China Special Postdoctoral Science Foundation (2020T130303), China
Postdoctoral Science Foundation (2019M661854), Postdoctoral Science Foundation of Jiangsu Province (2019K142), Qing Lan Project
of Jiangsu Province (2019), 333 Project Foundation of Jiangsu Province (BRA2018337), the Royal Society of New Zealand Catalyst
Seeding grant (CSG-FRI1901), the funding from the New Zealand Ministry of Business, Innovation and Employment (MBIE) in the
framework of the Strategic Science Investment Fund (C04X1703, Scion Platforms Plan) for part of financial support. We are grateful to
Dr. A. Dickson (Scion, New Zealand) and Dr. T. Singh (Scion, New Zealand) for their comments and suggestions.
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Sailing Zhu is currently working toward her Ph.D. under the supervision of Prof. Jingquan Han in College of Materials Science and Engineering at
Nanjing Forestry University (China). Her research interests revolve around the wood-based composite materials, including their processing, char
acterization, along with integration in flexible and wearable devices.
Subir Kumar Biswas received his Ph.D. (2019) in agricultural science (functional bio-based materials) from Kyoto University (Japan). Currently, he is
a postdoctoral researcher in Prof. Hiroyuki Yano’s group at Kyoto University. His interests cover wood nanotechnology including nanocelluloses and
the development of structurally hierarchical (nano)composites via hydrophilic-hydrophobic interaction of the components.
Zhe Qiu is currently pursuing his Ph.D. under the supervision of Prof. Yanjun Xie in College of Materials Science and Engineering at Northeast Forestry
University (China). Now, he is studying as a visiting student in Feng Jiang’s group in Department of Wood Science at the University of British
Columbia. His research interests focus on the wood-based functional materials, including wood modification, transparent wood, utilization of wood
structure and wood-based bionic materials.
28
Yiying Yue is currently an associate professor and a master supervisor in College of Biology and the Environment at Nanjing Forestry University
(China). She received her Ph.D. in Renewable Natural Resources at Louisiana State University (USA) in 2015. Her research interests cover environ
mental functional bio-based materials including photo-catalytic materials, filtering materials, oil/water separation materials, desalination materials
and intelligent detection materials etc.
Qiliang Fu received his PhD degree (2018) from the department of Fibre and Polymer Technology at KTH Royal Institute of Technology. He was
employed as a scientist at Scion (New Zealand Forest Research Institute Limited) in 2018-2022. Currently, he is a full professor in College of Materials
Science and Engineering at Nanjing Forestry University. Dr Fu carries out his independent research and focuses on wood nanotechnologies and
nanoscience, as well as wood-based nanocomposites and cellulosic functional nanomaterials.
Feng Jiang received his PhD degree in Macromolecular Science and Engineering from Virginia Tech in 2011. He is currently Assistant Professor in the
Department of Wood Science at the University of British Columbia, and Tier II Canada Research Chair in Sustainable Functional Biomaterials. He
serves as Editor of Carbohydrate Polymers and is the 2021 recipient of ACS CELL KINGFA Young Investigator Award. His research areas focus on
sustainable isolation and modification of lignocellulosic nanomaterials, as well as advanced manufacturing of bio-based products developments for
emerging thermal, environmental, electrical, and energy applications.
Jingquan Han received his Ph.D. in renewable natural resources from Louisiana State University (USA) in 2014. He is currently a Professor and Ph.D.
supervisor in College of Materials Science and Engineering at Nanjing Forestry University (China). His current research interests focus on the biomass-
based soft nanocomposite materials with sustainability, renewability and biocompatibility, including gels, elastomers, membranes, macro/nanofibers,
and their advanced applications in multifunctional wearable electronic devices.
29

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Progress in Materials Science 132 (2023) 101025

Contents lists available at ScienceDirect

Progress in Materials Science

Transparent wood-based functional materials via a

2. Transparency mechanism and processing methods

Delignified/PMMA Beech 0.1 70 2.5 150 ~10 [218]

Progress in Materials Science 132 (2023) 101025

Ply 0/90/0/-90/ Balsa 3.5 10 83 80 ~4.1 ~50.1 1.2 //

Lignin-retaining/thiol − Balsa 1.2 ~4.3 90 36 3.4 59 2.5

Progress in Materials Science 132 (2023) 101025

scalable manufacturing of larger-scale sustainable wood-based functional materials.

(caption on next page)

3.2.1. Optical properties

3.2.2. Mechanical properties

3.2.3. Thermal properties

3.3.1. Transparent and smart building materials: TWM as an alternative to glass

achieved with glass (Fig. 8f).

3.3.2. Optoelectronic devices: TWM as an alternative to plastics

5. Summary and future outlook

Declaration of Competing Interest

Data will be made available on request.

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