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different materials used will arise. When cellulose nanofibers
are dispersed uniformly enough throughout a transparent
polymer matrix, they can strengthen the polymer while the
resulting composite material retains its transparency.
[8–10]
Fol-
lowing that, Okahisa et al.
[11]
have succeeded in combining
organic light-emitting diodes (OLEDs) with optically trans-
parent wood cellulose nanocomposites.
However, nanofibers production is high in energy consump-
tion. Hence, we recently successfully fabricated transparent
nanocomposites using heterogeneous micro-scale chitin pow-
ders consist of uniform chitin nanofibers, in the first report
of nanostructured particle reinforced composites.
[12,13]
The
resulting material displayed high toughness and thermal sta-
bility at elevated temperatures. Encouraged by these findings,
we herein developed a low thermally expanded transparent film
by exploiting wood fibers that can be considered to be nano-
structured fibers in which individual nanofibers do not signifi-
cantly agglomerate and are orientated parallel to the fiber direc-
tion in S2 layer which accounts for 70–80% of wood fibers. We
thereby demonstrate that paper, used since ancient times, will
be a next-gen optical material.
The cell wall of wood has a fascinating 3D hierarchical
structure designed to maximize the stability and durability of
the tree. Wood fiber is made up of semi-crystalline cellulose
nanofibrils ( Figure 1), random amorphous hemicelluloses,
and lignin that cross-link the different polysaccharides in
wood to form a strong and durable structure.
[14]
Drying after
the removal of a matrix such as hemicellulose and lignin gen-
erates strong hydrogen bonding, causing aggregation between
the fiber bundles because the cellulose polymer molecules have
a linear chain structure consisting of repeating glucose units
with three hydroxyl groups. In the natural state, the delignified
fiber wall has a specific surface area of around 100 m
2
/g. The
fiber wall collapses during drying, decreasing the specific sur-
face area to around 1 m
2
/g.
[14]
This resulted in an opaque com-
posite when the matrix-removed wood pulp sheet was impreg-
nated into acrylic resin, due to light scattering.
Hence, generation of hydrogen bonding among cellulose
nanofibers in the wood pulp must be avoided.
[15]
In this study,
the wood pulps were acetylated with much care taken to main-
tain a never dried state. The degree of substitution (DS) value
of the wood pulp by the acetylation was 1.25 and the moisture
content of untreated wood pulp sheet at 23 °C and 50% relative
humidity (RH) decreased from 6.4% to 2.8% due to the treat-
ment. Acetylation also accelerated the filtration speed when
producing sheets due to the increased hydrophobicity of the
acetylated pulp fibers. The dried acetylated pulp sheets were
impregnated in acrylic resin (ABPE 10, refractive index 1.536
at 590 nm, Shin-Nakamura Chemical Co. Ltd) under vacuum
at a pressure of 0.01 MPa for 12 h. Both the acetylated and the
Wood Pulp-Based Optically Transparent Film: A Paradigm
from Nanofibers to Nanostructured Fibers
Hiroyuki Yano,* Shouzou Sasaki, Md. Iftekhar Shams, Kentaro Abe, and Takeshi Date
Prof. H. Yano, S. Sasaki, Prof. Md. I. Shams,
Dr. K. Abe, T. Date
Research Institute for Sustainable Humanosphere
Kyoto University
Uji, Gokasho, Kyoto, 611–0011, Japan
E-mail: yano@rish.kyoto-u.ac.jp
Prof. Md. I. Shams
Forestry and Wood Technology Discipline,
Khulna University
Khulna, 9208, Bangladesh
T. Date
Nippon Paper Industries Co., Ltd.
5–21–1 Oji, Kita-ku, Tokyo 114–0002, Japan
DOI: 10.1002/adom.201300444
In the digital era, ample information is being exchanged
through electronic media and the demand for high-quality,
smart, and portable digital devices is increasing sharply.
Because of its very low coefficient of thermal expansion,
7–10 ppm K
-1[1]
and transparency, glass has up to now been
used extensively in the substrates of electronic devices such as
displays and solar cells. However, in modern flat panel display
(FPD) technology and solar cell production, continuous “roll-
to-roll” (RTR) processing using flexible plastic substrates is
expected to take over from conventional “batch” processing of
glass substrates. Plastic is no doubt a good choice for flexible
displays and solar cells because it allows sufficient mechan-
ical and optical performance for these applications. However,
practical RTR processing has so far been prevented by the
high coefficient of thermal expansion (CTE) of the plastics to
be used. One possible way to reduce thermal expansion while
only causing a low loss in transparency would be to use fillers
with a diameter significantly smaller than the wavelength of
visible light.
[2]
Nanofibers are believed to have the potential to
substantially improve the mechanical properties of polymers
because their large interfacial area enables an applied load to
be transferred through filler/matrix interface while maintaining
transparency.
[3,4]
It is well known that different varieties of nanofibers can
be found in nature. Among them, cellulose nanofibers 4 to
20 nm in width, the major component of the plant cell wall
and the most abundant bio resources on earth, have received
great interest because of their outstanding mechanical proper-
ties due to their high molar mass and highly ordered extended
chain polysaccharide nanofiber structures. The maximum
macroscopic Young's modulus of plant cellulose is 128 GPa,
[5]
and the elastic modulus of the crystalline regions of cellulose I
is 138 GPa.
[6]
Surprisingly, its coefficient of thermal expansion
in the axial direction is as low (0.1 ppm K
-1
) as that of quartz.
[7]
This makes it a preferable candidate for RTR manufacturing
processes because no discrepancy between the CTEs of the
Adv. Optical Mater. 2014, 2, 231–234