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Dried-state bacterial cellulose ( Acetobacter xylinum ) and polyvinyl-alcohol-

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 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx

Contents lists available at ScienceDirect

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Original Article

Dried-state bacterial cellulose (Acetobacter xylinum) and polyvinyl-alcohol-based

hydrogel: An approach to a personal care material
N. Chunshoma, P. Chuysinuanb, S. Techasakulb, S. Ummartyotina, ∗

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a
Materials and Textile Technology, Faculty of Science and Technology, Thammasat University, Patumtani, Thailand
b
Laboratory of Organic Synthesis, Chulabhorn Research Institute, Bangkok, Thailand

ARTICLE INFO ABSTRACT

Article history: Freeze-dried bacterial cellulose and polyvinyl alcohol were successfully prepared. The weight ratios of

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Received 1 May 2018 polyvinyl alcohol to bacterial cellulose were set at 3:1, 5:1 and 10:1. With bacterial cellulose present in the
Received in revised form 15 June 2018 polyvinyl alcohol matrix, H-bonds formed along the cross-linked hydrogel network. The freeze-dried hydro-
Accepted 23 June 2018
gel presented good compatibility. The hydrogel was thermally stable up to 200 °C. Scanning electron mi-
Available online xxx
croscopy showed that the hydrogel presented an interconnected network containing various pore sizes. Pre-
liminary experiments on the swelling behavior of the hydrogel were done in DI water, an NaCl solution and a
Keywords: PBS solution. The hydrogel showed good swelling characteristics within 30 min. Importantly, the freeze-dried
Bacterial cellulose hydrogel is an excellent candidate for pharmaceutical and cosmetic materials.
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Freeze dried hydrogel © 2018.
Poly vinyl alcohol

1. Introduction However, to use only neat poly(vinyl alcohol) was still in trouble.
It affected on cell affinity and consequently caused the rejection due
In recent year, the development of hydrogel has been extremely to weak adhesion. To solve this issue, the design of poly(vinyl alco-
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developed for significant interest in biomedical fields. Utilization of hol) based composite was considered as alternative technique. To de-
hydrogel based materials gained much attractive to be the candidate sign composite, bacterial cellulose was considered as an effective re-
because of distinctive properties and benefit of exhibiting the charac- inforcement. From the structural point of view, it was composed of
teristics similar to soft biological tissues [1]. Due to the evidence in nano-sized fibril network. It was free from wax, lignin and hemicel-
viscoelastic properties, high water content, the role of hydrogel was lulose. Moreover, it provided high tensile strength, low co-efficient of
employed in various medical researches such as bone and cartilage thermal expansion as well as high chemical stability. Bacterial cellu-
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repair, drug delivery system, cosmetic as well as contact lens. From lose was therefore considered as a filler to design polymer based com-
the fundamental point of view, hydrogel can be divided into chem- posite [6–8].
ical gels and physical gels. It can be defined that physical gel was In an attempt to increase the properties of poly(vinyl alcohol)
formed by molecular self-assembly through ionic or hydrogen bond, based composite for hydrogel, many scientists found that bacterial
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while chemical gel was formed by covalent bond [2]. Up to the present cellulose can be used as reinforcement material for poly(vinyl alco-
time, numerous polymers have been extensively investigated on the hol) based hydrogel. Wang et al. [9] investigated the preparation and
feasibility to become hydrogel. One of the most interests was focused in vitro characteristic of bacterial cellulose and poly(vinyl alcohol) hy-
on poly(vinyl alcohol). It was considered as a well-known synthetic drogel composite. Gao et al. [10] exhibited that the role of bacterial
polymer ascribed to its desirable characteristics such as water-soluble, cellulose in hydrogel network provided the effect on mechanical and
nontoxic, transparent as well as biocompatible. Our research group rheological properties. This effect was related to numerical prediction
has successfully developed poly(vinyl alcohol) for drug delivery sys- [11]. Furthermore, Wang et al. [12] also found that the role of cellu-
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tem [3,4]. It was found that poly(vinyl alcohol) presented the excel- lose in hydrogel network presented the self-healing and antibacterial
lent properties such as chemical stability and water-uptake capability. properties.
Moreover, we extent the scope of work for gelatin based composite, Although bacterial cellulose and poly(vinyl alcohol) based com-
utilization of gelatin based hydrogel also provided the good benefit posite presented many advantages such as significant enhancement of
such as cost effective and degradability [5]. mechanical properties and thermal stability, it was still limited for the
service life time of product. Water in 3D network of hydrogel can
cause a media for fungal and microbial specie. As a consequence, the
utilization of hydrogel was therefore limited. In order to use poly(vinyl
Peer review under responsibility of Vietnam National University, Hanoi. alcohol) based hydrogel with higher efficiency, freeze-dried hydro-
∗
Corresponding author. Fax: +66 25644458. gel was considered as one of the most effective routes for
Email address: [Link]@[Link] (S. Ummartyotin)

[Link]
2468-2179/ © 2018.
2 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx

utilization. In 2016, Butylina et al. [13] investigated the properties of 2.2. Methods
as-prepared and freeze-dried hydrogel made from poly(vinyl alcohol)
and cellulose. With pouring water to freeze-dried hydrogel, it was 2.2.1. Bacterial cellulose extraction and purification
swelled and ready to use. Also, it was facilitated on design of pack- Bacterial cellulose was extracted from nata de coco, which was
aging and logistic which was considered on lightweight of product. rinsed with distilled water to remove excess sugar and blended in a
Utilization of dried-state of hydrogel prepared from bacterial cellulose laboratory blender to obtain nata de coco pellicles. These pellicles

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and poly vinyl alcohol can be provided many benefits including light- were treated with 0.1 M NaOH at 80 °C for 1 h to remove any re-
weight, packaging design as well as storage. One of the most impor- maining microorganisms, medium components, and soluble polysac-

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tant applications is focused on personal care cosmetic and treatment. charides. The purified bacterial cellulose was then thoroughly washed
The use of dried hydrogel has extensively been attractive for personal with distilled water until a neutral pH was achieved.
care material such as cleansing mask and moisturizer. Further appli-
cation may extend to ingredient of skincare product, which was com- 2.2.2. Preparation of freeze-dried bacterial cellulose and poly (vinyl
monly employed in dairy. alcohol) composite
In this research work, we wish to present the physico-chemical Bacterial cellulose and poly (vinyl alcohol) based composite was
properties of freeze-dried hydrogel prepared from poly(vinyl alco- prepared as hydrogel form and freeze-dried powder. To achieve this,
hol) and bacterial cellulose based composite. Morphological, thermal, 10 wt% of poly (vinyl alcohol) was completely dissolved in water, and

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and structural properties of freeze-dried hydrogel composite were pre- then a bacterial cellulose suspension was poured into the poly (vinyl
sented. Preliminary investigation on swelling behavior was observed. alcohol) solution. Borax was employed as a crosslinking agent. The
reaction was performed at 70 °C for 4 h. The chemical reaction that
occurred between the bacterial cellulose and poly (vinyl alcohol), with
2. Experimental 1 wt% of disodium tetraborate, is exhibited in Fig. 1. Subsequently,
the hydrogel composite was washed with deionized water to remove
2.1. Materials any unreacted chemicals and stored at 4 °C. In this experiment, neat

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poly (vinyl alcohol) was also studied for comparison. The ratios of
Bacterial cellulose was successfully extracted from Nata de coco poly (vinyl alcohol) and bacterial cellulose were set as 3:1, 5:1 and
product (Chaokoh coconut gel in syrup, Ampol Food Processing Ltd., 10:1 respectively.
Nakornpathom, Thailand). An indigenous dessert of which main com- To prepare freeze-dried poly (vinyl alcohol) and bacterial cellu-
ponent was reported as bacterial cellulose. Characterizations of bacte- lose composite, the as-prepared hydrogel composite was undergone
rial cellulose extracted from Nata de coco were carried out in previ- freeze-dry process. Drying condition were temperature of −50 °C,
ous work; its characteristics matched those of bacterial cellulose ex- vacuum of 0.12 mbar for 7 h. After freeze-dry process, the sample was
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tracted from the culture of Acetobacter Xylinum [6–8]. On the other kept in desiccator in order to prevent the moisture adsorption.
hand, poly(vinyl alcohol), sodium hydroxide were purchased from
Ajax Fine-chem, Co. LTD Thailand. The average of molecular weight 2.2.3. Investigation of swelling behavior of freeze-dried bacterial
was estimated to be 10 000 g/mol. Disodium tetraborate with a mole- cellulose and poly vinyl alcohol based hydrogel composite
cular weight of 381 g/mole was also purchased from Ajax Fine-Chem The as freeze dried bacterial cellulose and poly vinyl alcohol hy-
Co. LTD Thailand. All chemical reagents were used as received with- drogel composite was investigated on swelling behavior and gel frac-
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out further purification. tion. In this study, the gravimetric technique was employed to deter-
mine the swelling and equilibrium data of the hydrogel. It was im-
mersed in DI water, 0.1 NaCl solution and PBS solution for 3 h. After
an appropriate time interval, specimens were removed from the solu
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Fig. 1. Schematic diagram of as freeze dried poly(vinyl alcohol) and bacterial cellulose hydrogel composite preparation.
 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx 3

tion, dried with a filter paper to remove excess solvent, and were mea- 2.3.4. X-ray diffraction
sured. Five samples were investigated, and the data were reported as The crystal structure of the freeze dried hydrogel composite was
the statistical average and standard deviation. The swelling ratio was investigated by X-ray diffraction (XRD, Phillips P.W. 1830 diffrac-
determined as follows (Eq. (1)): tometer), which was employed using nickel-filtered CuKa radiation.
The diffraction patterns were recorded over a range of 10°–80°.

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(1) 2.3.5. Differential scanning calorimetry
DSC of the freeze dried hydrogel composite was performed from

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where Wwet is the weight of a swollen hydrogel at submersion time, room temperature to 400 °C at a heating rate of 10 °C/min with a
and Wdry is the initial weight of the dry hydrogel. TA-10000 DSC (TA Instruments, DE, USA). The aluminum pan is
used for sample holder. The glass transition temperature, melting tem-
perature, and specific heat capacity were determined from the heat
2.3. Instruments flow curve.

2.3.1. Thermogravimetric analysis 3. Results and discussion

The thermal degradation behavior of the freeze dried hydrogel

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composite was characterized using TGA (TGA Q500, TA Instru- 3.1. Physico-chemical properties of freeze-dried hydrogel composite
ments). In total, 20 mg of the sample was heated from room tempera- prepared from bacterial cellulose and poly vinyl alcohol
ture to 700 °C in N2 at a heating rate and a flow rate of 5 °C/min and
70 ml/min, respectively. Freeze dried hydrogel composite was prepared from bacterial cel-
lulose and poly vinyl alcohol. Fig. 2 presents FTIR spectra of
2.3.2. Scanning electron microscopy freeze-dried hydrogel composite. The characteristic absorption bands
The freeze dried hydrogel composite was investigated using SEM at 1100 cm−1 and 1750 cm−1 were attributed to C O stretching and

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(SEM, Quanta 250 microscope, Japan). The specimens were C O stretching, respectively. It was referred to poly vinyl alcohol.
gold-coated using a sputtering device (Jeol, JFC-1200) prior to the With the existence of bacterial cellulose, the characteristic cellulose
SEM observation. A magnification of 1000× was used. signals of C O C pyranose ring skeletal vibration at 1050 cm−1
was observed. This was similar to previous article reported by Lin
2.3.3. Fourier transform infrared spectroscopy et al. [14]. It can be implied that the characteristic peak of poly vinyl
FTIR spectra were recorded using a Fourier transform infrared alcohol was slightly shifted toward with that of cellulose in the com-
spectrometer (PerkinElmer, USA). Spectra were measured at room posites samples. The characteristic peak at 2900 cm−1 was attributed
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temperature in the spectral range from 4000 to 400 cm−1 with a reso- to C H stretching of both bacterial cellulose and poly vinyl alcohol.
lution of ±4 cm−1 and a scan frequency of 32 times. The O H stretching was due to hydrophilic surface.
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Fig. 2. FTIR pattern of freeze-dried hydrogel composite.

4 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx

Fig. 3 presents the crystal structure of freeze-dried hydrogel com- into three different regions. From room temperature to 300 °C, the
posite. Without the water, it was important to note that XRD patterns thermal decomposition was involved on water evaporation, approx-
exhibited crystalline peak at 2θ = 23° corresponding to (200) crys- imately 10 %wt of weight loss was observed, suggesting that the
tal plane, which was coincided with the result reported by Yan et al. weight loss was ascribed to the loss of free and bound water. It was
[15]. When bacterial cellulose has been inserted into freeze-dried poly important to note that freeze-dried hydrogel was easily to adsorb mois-
vinyl alcohol based composite, the intensity of bacterial cellulose peak ture. This discussion has been consistent with previous article re-

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was significantly observed. It can be suggested that the relative de- ported by Qi et al. [16]. After that, with the increment on tempera-
gree of crystallinity of freeze-dried hydrogel composite was signifi- ture to 300–500 °C, the weight loss was attributed to decomposition

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cantly increased. The role of bacterial cellulose in freeze-dried hydro- of poly vinyl alcohol and bacterial cellulose. The decomposition curve
gel composite provided the good effectiveness in mechanical and ther- of the neat poly vinyl alcohol was shifted toward a slightly higher
mal properties. The amorphous region of poly vinyl alcohol was re- temperature. This also indicated that with the existence of bacterial
duced due to addition of bacterial cellulose. It can be implied that there cellulose, composite presented higher thermal stability as suggested
is an occurrence reaction between poly vinyl alcohol and bacterial cel- by Saba et al. [17]. Bacterial cellulose has high melting temperature
lulose. and it was consequently provided high thermal stability for compos-
Fig. 4 exhibits the thermal decomposition of freeze-dried hydro- ite. It was notable that both poly vinyl alcohol and composite exhib-
gel composite. Neat poly vinyl alcohol was provided for comparison. ited two steps of degradation. From temperature of 300–400 °C, the

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Thermal decomposition of freeze-dried hydrogel can be categorized weight loss was due to the elimination of the residual water trapped
in the poly vinyl alcohol and bacterial cellulose. With the temperature
region of 400–500 °C, it was involved on the decomposition of both
poly vinyl alcohol and bacterial cellulose. They changed to CO2. The
evaporation of water and CO2 has been observed as pathway of evap-
oration. It presented as a porous structure. With the temperature above
500 °C, the decomposition was terminated. 10–20 %wt of yield was

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observed as a residual. It can be also implied that with the existence
of bacterial cellulose, higher percent yield of residual was observed,
suggesting that bacterial cellulose provided higher thermal stability to
composite. From TGA curve, it can be concluded that no change on
thermal stability on utilization of freeze-dried hydrogel at room tem-
perature was observed.
Fig. 5 exhibits the DSC curves of freeze-dried hydrogel compos-
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ite. It was important to note that the glass transition temperature of
neat poly vinyl alcohol was estimated to be 70 °C, which was very
much close to the reported value (about 68 °C) [18]. With the exis-
tence of bacterial cellulose, the glass transition temperature of poly
vinyl alcohol based composite was slightly shifted to higher value. It
can be implied that strong interaction between bacterial cellulose and
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Fig. 3. XRD pattern of freeze-dried hydrogel composite.

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Fig. 4. Thermal stability of freeze-dried hydrogel composite.

 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx 5

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Fig. 5. DSC thermogram of freeze-dried hydrogel composite.

poly vinyl alcohol was occurred as suggested by Jipa et al. [19]. In 3.2. Swelling properties of freeze-dried hydrogel composite prepared
addition, the melting temperature of freeze-dried hydrogel composite from bacterial cellulose and poly vinyl alcohol
was investigated. The endothermic peak was estimated to be 320 °C.
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This temperature can be used to explain conformational change within Fig. 7 presents the swelling behavior of as freeze-dried bacterial
the polymer network. It may involve the size of the crystallites and cellulose and poly vinyl alcohol based hydrogel composite. The ex-
the degree of crystallinity as suggested by Hassan et al. [20]. It was periment was set up based on swelling behavior on DI water, 0.1
remarkable to note that to compare with neat poly vinyl alcohol; the NaCl solution and PBS solution, respectively. From the fundamen-
melting point of composite was slightly shifted to higher. It could tal point of view, lesser cross-linked hydrogel exhibited higher wa-
be attributed to the dissociation process of inter- and intra-hydrogen ter uptake ability, due to the highly cross-linked structure could not
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bonding between bacterial cellulose and poly vinyl alcohol. The in- sustain much water within hydrogel structure. In our experiment, neat
crement on melting temperature of composite indicated that the incor- poly vinyl alcohol was provided for comparison. It was remarkable
poration of bacterial cellulose weakened the interaction between poly that poly vinyl alcohol was easily to dissolve in three different media.
vinyl alcohol chain and hindered the crystallization of poly vinyl alco- With the existence of bacterial cellulose, the swelling behavior of as
hol. This discussion was strongly in agreement with XRD pattern. freeze dried hydrogel was determined. This phenomenon was attrib-
Fig. 6 depicts the SEM image of cross-section morphological prop- uted to the hydrophilic nature of bacterial cellulose and poly vinyl al-
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erties of freeze-dried bacterial cellulose and poly vinyl alcohol based cohol [22]. However, with the increment on the fraction of bacterial
hydrogel composite. It was important to note that hydrogel composite cellulose, the decrease on the swelling behavior of as freeze dried hy-
exhibited an interconnected porous structure with regular pore distri- drogel was probably occurred due to the reinforcing effect of the bac-
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bution. The average pore size declined with increment on poly vinyl terial cellulose. It was considered as nano-reinforcing element in poly
alcohol content. The pore size was therefore ranging from 10 μm to vinyl alcohol matrix, restraining the swelling mechanically resulting
100 nm. Various pore sizes trend provided a better explanation to the in a decrease on water and solvent adsorption at higher bacterial cel-
swelling capacity and water evaporation characteristic of freeze-dried lulose addition level. This discussion was strongly agreed with pre-
hydrogel composite. With the existence of bacterial cellulose, the vious literature reported by Naizi et al. [23]. Comparison to different
physical crosslinking density of the hydrogel composite increased, solution, the swelling behavior of as freeze dried bacterial cellulose
leading to the water content of hydrogel composite decreased. How- and poly vinyl alcohol hydrogel was less. It was due to less amount
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ever, from the fundamental point of view, in freeze dry process, free of free ion in solution. The hypothesis of swelling behavior in differ-
water was frozen into larger ice crystals which were eventually rep- ent solution was set up based on ionic strength of medium had a vital
resented by larger pores. This discussion was in agreement with pre- influence on the swelling capabilities of as freeze dried bacterial cel-
vious article reported by Dinu et al. [21]. These results were consid- lulose and poly vinyl alcohol hydrogel. It may involve in interaction
ered as an important relationship in the tuning of the size distribu- either through surface adsorption or hydrogen bonding between bac-
tion, which can facilitate permeation of cellular growth factor when terial cellulose and poly vinyl alcohol as suggested by Mandal et al.
freeze-dried hydrogel composite will be employed as medical mater- [24]. It was important to note that only in DI water, the swelling be-
ial. havior was significantly less. DI water is in neutral pH and there is no
ion to adhere on the functional group of bacterial cellulose and poly
6 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx

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Fig. 6. SEM micrograph of freeze-dried hydrogel composite (A) neat poly vinyl alcohol (B) 3:1 ratio of poly vinyl alcohol and bacterial cellulose (C) 5:1 ratio of poly vinyl alcohol
and bacterial cellulose (D) 10:1 ratio of poly vinyl alcohol and bacterial cellulose.
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vinyl alcohol based hydrogel. Compare to 0.1 NaCl and PBS solu- tron microscope. The high amount of bacterial cellulose in hydrogel
tion, there are positive and negative free ions in solution, it conse- composite can form the interaction between poly vinyl alcohol net-
quently dissolved and adhered on the functional group of bacterial cel- works, suggesting that high gel fraction can be obtained. No obvious
lulose and poly vinyl alcohol based hydrogel. Higher swelling ratio change in crystallinity of hydrogel was found after addition of bac-
was therefore observed. terial cellulose. It was remarkable to note that for potential biomed-
ical application of hydrogel, it presented the excellent characteristic in
4. Conclusion high water absorption. Utilization of freeze dried hydrogel can be ben-
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eficial for design and point of care product for patient. It should be fur-
In this study, physico-chemical properties of as-freeze dried bac- ther employed and developed for pharmaceutical technology and cos-
terial cellulose and poly vinyl alcohol was investigated. It was found metic product.
that properties of as freeze dried hydrogel can be modified by addi-
tion of bacterial cellulose into poly vinyl alcohol network. The ratio
of 3:1 between poly vinyl alcohol and bacterial cellulose presented Acknowledgment
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the outstanding characteristic on swelling behavior. Freeze dry tech-

nique was used to remove water from hydrogel network. It resulted in The authors would like to acknowledge the financial support pro-
shrinkage of hydrogel composite. The existence of bacterial cellulose vided by Thammasat University. We are grateful for the space and re-
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played an important effect on pore size as observed by scanning elec search facilities support by the Chulabhorn Research Institute. Special
thank was extent to Plastic Institute of Thailand.
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 Journal of Science: Advanced Materials and Devices xxx (2018) xxx-xxx 7

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