Properties of bacterial cellulose transparent
film regenerated from dimethylacetamide–LiCl
solution
R. Yudianti
a
*, A. Syampurwadi
a
, H. Onggo
a
, M. Karina
a
, H. Uyama
b
and
J. Azuma
b
Excellent transparent films were prepared from bacterial cellulose (BC) sheets by solubilization of its defibrillated
freeze-dried specimens in a solvent of dimethylacetamide (DMAc) containing 8.0% (w/w) lithium chloride (LiCl),
and their properties were compared with those of the native BC. Fibrillar structure of the native BC disappeared after
dissolution, and the film formed after dissolution also loose this structure. Occurence of structural transformation
from crystalline to amorphous state was also evidenced by X-ray diffraction, solid state cross polarization/magic an-
gle spinning
13
C-NMR and attenuated total reflectance–Fourier transform infrared spectroscopic analyses. In addi-
tion, excellent 3D uniform structure of the transparent BC film was further evidenced by X-ray micro computed
tomography. Plastic-like characteristic was enhanced by film formation after dissolving the BC specimens in the
DMAc–LiCl solution as shown by changing mechanical properties, a slight decrease in tensile strength (67.2 to
59.6 MPa) and breaking stress (67.2 to 58.4 MPa) but significant increase in elongation at break from 3.4 to 10.5%,
and improvement of work of fracture from 5.8 to 21.2 kJ/m
2
. Copyright © 2016 John Wiley & Sons, Ltd.
Keywords: bacterial cellulose; transparent film; DMAc–LiCl solution
INTRODUCTION
Bacterial cellulose (BC) is a typical natural cellulose which has a
unique gel-sheet structure having I
α
crystalline polymorph in
comparison with plant cellulose rich in I
β
crystalline poly-
morph.
[1,2]
Because of high crystallinity, tensile strength and elas-
tic modulus, its compatibility, and mixing ability with other
materials are becoming promising factors for its use as a func-
tional material. Previously, various kinds of modification of BC
were tried
[3]
and bio-compatible films was also prepared.
[4]
We
have succeeded to prepare a new type BC sheet modified selec-
tively at one side of the sheet with introduction of aldehyde
groups at O-6, and suggested the importance of the surface
structure for its mechanical strength.
[5]
Potential of BC as a functional material could further be in-
creased by its solubilization to make transparent film. Yano
et al. discovered that BC nanofiber had very promising character-
istic as reinforcing material for optically transparent plastic.
[6]
Dissolution of cellulose in solvent is a keyprocess for making
composite with other materials. For further application, conduc-
tive transparent BC could be able to contribute for many optical-
electronic devices such as organic light emitting diodes, organic
photovoltaic solar cells, liquid crystal display panels, and touch
panels. The most critical requirements for transparent conduc-
tive film or glass are low sheet resistance and high
transparency.
[7]
Recently, Zhang et al. developed a method for preparation of
amorphous cellulose films with excellent transparency from
dimethylacetamide (DMAc)–lithium chloride (LiCl) solutions by
using acetone as the regeneration solvent.
[8]
Although applica-
bility of this method to BC is briefly mentioned in this report,
no detailed description was explained by using the BC sheets
usually prepared in Southeastern Asia countries including
Indonesia. Matsumoto et al. also reported that the solution of
BC in the DMAc–LiCl exhibits optical anisotropy and has a differ-
ent viscosity behavior from plant origin celluloses,
[9]
but did not
refer to the film formation.
On account of dissolution mechanism of cellulose in the
DMAc–LiCl solution, a lot of works
[10–18]
have been performed
since the first report of this solvent by McCormick and
Lichatowich.
[19]
A generally accepted dissolution process was
demonstrated as formation of [DMAc
n
+ Li]
+
macrocation by in-
teraction of Li
+
cation with carbonyl group oxygens of DMAc
molecules, with concomitant formation of strong hydrogen
bonds between hydroxyl protons of cellulose and Cl
À
anion ac-
companied by splitting of hydrogen bonded networks of cellu-
lose, followed by dispersion of cellulose chains. Notable
characteristics of this solvent are in that the solvent does not
form chemical bonds with the cellulose molecule and Li
+
and
Cl
À
ions behave as an ion pair. Previously, the process for activa-
tion of cellulose from paper substrates by solvent exchange nec-
essary to solubilize it was also optimized to follow with a
* Correspondence to: Rike Yudianti, Indonesian Institute of Sciences, Research
Center for Physics, Jalan Cisitu No. 21/154D, Bandung, West Java, 40135,
Indonesia.
E-mail: rikeyudianti@yahoo.com; rikeyudianti@gmail.com
a R. Yudianti, A. Syampurwadi, H. Onggo, M. Karina
Research Center for Physics, Indonesian Institute of Science, Bandung,
Indonesia
b H. Uyama, J. Azuma
Graduate School of Applied Chemistry, Osaka University, Osaka, Japan
Research article
Received: 11 November 2015, Revised: 11 January 2016, Accepted: 28 January 2016, Published online in Wiley Online Library
(wileyonlinelibrary.com) DOI: 10.1002/pat.3782
Polym. Adv. Technol. (2016) Copyright © 2016 John Wiley & Sons, Ltd.