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Food Hydrocolloids 93 (2019) 276–283

Contents lists available at ScienceDirect

Food Hydrocolloids
journal homepage: www.elsevier.com/locate/foodhyd

A simple method for improving the properties of the sago starch films T
prepared by using ultrasonication treatment
Hairul Abrala,∗, Azmi Basria, Faris Muhammada, Yuzalmi Fernandoa, Fadli Hafizulhaqa,
Melbi Mahardikaa, Eni Sugiartib, S.M. Sapuanc, R.A. Ilyasc, Ilfa Stephaned
a
Department of Mechanical Engineering, Andalas University, 25163, Padang, Sumatera Barat, Indonesia
b
High-Temperature Coating Laboratory, Research Center for Physics, Indonesian Institute of Sciences (LIPI), Serpong, Indonesia
c
Department of Mechanical and Manufacturing Engineering, Faculty of Engineering, Universiti Putra Malaysia, 43400, UPM Serdang, Selangor, Malaysia
d
Department of Information System, STMIK Indonesia Padang, 25136, Indonesia

A R T I C LE I N FO A B S T R A C T

Keywords: Starch granules containing amylopectin-rich fractions like sago starch may remain insoluble and undamaged
Starch film decreasing properties of the film. The aim of this study is to characterize native sago starch films prepared using
Transparency ultrasonication. An ultrasonication probe was used during gelatinization for 2.5, 5, and 10 min respectively.
Ultrasonication Ultrasonication decreases the incomplete gelatinized granules resulting in a film with a more compact structure,
Ghost
and lower moisture vapor permeability than non-treated film. The longest duration resulted in a film with the
highest transparency, and the highest thermal resistance. The duration for 5 min increased tensile strength of the
film by 227%, and its moisture absorption decreased by 29.83% compared to non-sonicated film. After ultra-
sonication for 10 min, melting temperature increased by 7% in comparison to non-sonicated film. This work
promotes a simple method to improve the tensile and physical properties of starch based film.

1. Introduction waves which shatter the aggregations of the agglomerated granules


suspended (Syafri, Kasim, Abral, & Asben, 2018).
Development of starch-based bioplastics has been given consider- Physical and mechanical properties of a maize starch film after ul-
able attention as an environmentally friendly biodegradable alternative trasonication of the starch gel improve due to an increase in homo-
to hydrocarbon-based plastics (Abral et al., 2018). When starch films geneity of the structural starch film resulting in increased transparency
are used for food packaging it is required to have good transparency, and tensile strength of the film along disappearance of the ghosts (Abral
sufficient strength and low moisture absorption so as be able to improve et al., 2018; Cheng, Chen, Liu, Ye, & Ke, 2010). In contrast, another
the shelf life of food. Solution casting is one of common method for previous study claimed that a high ghost phase fraction enhanced the
preparing starch film, especially at the laboratory level. During this tensile (elongation at break and tensile stress) properties of corn starch
preparation, some defects resulting in inhomogeneous structures may film (Garcia-Hernandez et al., 2017). These dissimilarities in results
occur. These inhomogeneous structure result from incompletely soluble could be due to differences in the starch sources used for preparing
starch granules often called ghosts (Abral et al., 2018). This can de- starch films.
crease the transparency of starch film (Garcia-Hernandez, Vernon- This present study used sago starch granules from Metroxylon Sagu
Carter, & Alvarez-Ramirez, 2017). Ghost formation is a result of cross- palm. This material is abundantly available in tropical country like
linking of polysaccharide chains within swollen granules (Debet & Indonesia and has a very low cost compared with other common star-
Gidley, 2007). Previous studies found that ultrasonication is effective in ches (Abral, Kasmianto, & Mastariyanto Perdana, 2012; Nouri &
reducing insoluble and agglomerated starch granules (Abral, Putra, Mohammadi Nafchi, 2014). Sago palm contains a large amount of
Asrofi, Park, & Kim, 2018; Lima & Andrade, 2010). This is because starch in its trunk and its productivity was about 4 times that of paddy
sound energy from ultrasonication produces acoustic cavitation: the rice (Karim, Tie, Manan, & Zaidul, 2008). Sago starch has unique
formation, growth, and collapse of starch granules within the liquid characteristics and some of its physicochemical properties similar to
matrix (Asrofi et al., 2018b; Mahardika, Abral, Kasim, Arief, & Asrofi, common starch like cassava and potato (Mohammadi Nafchi, Cheng, &
2018). The violent collapse of the bubbles results in microjets and shock Karim, 2011). It is a potential source for bioplastics with high


Corresponding author.
E-mail address: abral@ft.unand.ac.id (H. Abral).

https://doi.org/10.1016/j.foodhyd.2019.02.012
Received 14 August 2018; Received in revised form 24 January 2019; Accepted 6 February 2019
Available online 10 February 2019
0268-005X/ © 2019 Elsevier Ltd. All rights reserved.
H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

amylopectin content leading to better tensile properties (Ismail & Table 1


Zaaba, 2012). However, starch films from granules with high amylo- Viscosity of the starch gel before and after ultrasonication.
pectin may have incompletely soluble and agglomerated starch gran- Sample Viscosity (MPa.s) Rotation speed (rpm)/T (oC)
ules decreasing film properties (Debet & Gidley, 2007).
Many studies have been reported on the properties of starch-based S-0 4999 6/50
S-2.5 125
films made from various starches including high amylopectin corn, ji-
S-5 164
cama, and wheat (Abral et al., 2018; Debet & Gidley, 2007; Garcia- S-10 465
Hernandez et al., 2017; Hafizulhaq, Abral, Kasim, Arief, & Affi, 2018).
However, as far as the authors are aware no work has been reported on
sago starch film prepared using an ultrasonic probe. Therefore, the 2.3. Characterization
objective of the present study was to determine the properties of the
sago starch prepared by a simple and environmentally friendly method 2.3.1. Opacity
using ultrasonication further. The main motivation was to obtain the The opacity of the film was measured using UV-vis spectro-
optimum ultrasonic duration of the sago starch gel to maximize several photometer (Shimadzu UV 1800; Japan) between wavelengths of
properties of the film. Morphology of the fracture surface of the plas- 400–800 nm according to ASTM D 1003-00 (Standard Test Method for
ticized sago film was observed using a field-emission scanning electron Haze and Luminous Transmittance of Transparent Plastics). Films of
microscopy (FESEM). X-ray diffraction (XRD) and Fourier transform 0.34 mm thickness were cut into 9 × 35 mm rectangles. The opacity
infrared (FTIR) of films were characterized. Other properties measured measurement was carried out in triplicate.
are viscosity, transparency, tensile strength and modulus, fracture
strain, moisture absorption, water vapor permeability, and thermal 2.3.2. FESEM observation
resistance. The fracture surface of the sample after tensile testing was observed
using FESEM. The film samples were placed on the FESEM sample stub.
2. Materials and experiment They were coated with carbon and gold to reduce the static charge. The
surface morphology of the sample was observed using a model JFIB
2.1. Material 4610 SEM from JEOL with 10 kV and 8 mA.

Sago starch was obtained from local small-scale industry in Padang, 2.3.3. FTIR
Indonesia. For purification, the starch (1000 g) was mixed with distilled FTIR spectra of the non- and sonicated film (S-0, S-2.5, S-5, and S-
water (3000 mL). The solution was stirred manually for a 1 min. After 10) were recorded using an IR spectrometer (PerkinElmer Frontier
15 h, the liquid fraction containing purities was decanted off leaving equipment) to compare the functional groups and molecular bond
purer sediment of starch. This was repeated three more times. The re- structure of the film. Before the characterization, all samples were dried
sulting wet pure starch was poured into a Teflon plate to be dried in a using a drying oven (Universal Oven Memmert UN-55 at 50 °C) until
drying oven (Universal Oven Memmert UN-55) for 20 h at 50 °C. A constant weight. The dried samples were cut (approximately
small electrical blender was used to refine dried starch bundles for 10 × 10 mm) with steel scissor, formed into a sheet film and scanned at
5 min. Chemical analysis indicated that the purified sago starch con- a frequency range of 4000–600 cm−1 at 4 cm−1 resolution. Three dif-
tained 21% amylose, and 79% amylopectin indicating it was a high ferent locations for each sample per treatment were tested.
amylopectin content starch (Al-Hassan & Norziah, 2012).
2.3.4. X-ray diffraction
PANalyticalXpert PRO at 25 °C, 40 kV and 30 mA was used to per-
2.2. Preparation of the bioplastic
form X-ray diffraction testing. The samples were scanned from 2θ = 3°
to 40°. The crystallinity index (CI) percentage was measured using an
The purified sago starch, distilled water, and glycerol were weighed
Eq. (1) (Segal, Creely, Martin, & Conrad, 1958):
for 15, 150, and 7.5 g respectively using a precision balance to the
nearest 0.1 mg (Kenko). These materials were mixed and gelatinized (I200 − Iam)
CI (%) = x 100
using a hot plate magnetic stirrer (Daihan MSH-20D) at 500 rpm, 70 °C I200 (1)
for 45 min. This gelatinization temperature of sago gel was determined
by using a temperature probe integrated with the hot plate magnetic where I200 is the intensity of the peak at 22.6° which is associated with
stirrer. When the solution started to gelatinize that was the temperature the crystalline region of cellulose, and Iam is the intensity taken at
chosen for this process and subsequent ultrasonication. During gelati- 2θ = 18° in the diffraction pattern as characteristic of the amorphous
nization, four gel samples were treated; one without and three with regions in the cellulose.
ultrasonication for 2.5, 5, and 10 min respectively using a 20 mm dia-
meter SJIA 1200W ultrasonic probe at 600 W at 100% amplitude and 2.3.5. Tensile properties
20 kHz. Ultrasonication times longer than 10 min were initially trailed A testing machine (Com-Ten testing machine 95T) was used to
but because the of films from these proved too brittle for further testing characterize the tensile properties of films including tensile strength
so were not used in this study. Ultrasonic warming was limited so the (TS), tensile modulus (TM) and fracture strain (FS). All samples were
gel temperature did not exceed 70 °C. Viscosity of four non- and soni- prepared with ASTM D882-12 standard and conditioned for 48 h with
cated gel samples was measured using an NDJ-8S digital rotary visc- 50 ± 5% relative humidity at 25 °C. Tensile tests were performed with
ometer at 50 °C with rotor #2 at 6 rpm about 10 s. The sample was cast tensile speed for 3 mm/min at room temperature and repeated five
in a petri dish (140 mm diameter). The petri dish was vibrated using an times for each sample.
ultrasonic bath (PS-70AL, 420 W, 40 kHz, 100% amplitude) for 15 min
to remove trapped air bubbles and ensure homogeneity of the gel. A 2.3.6. Thermogravimetry analysis (TGA) and derivative (DTG), differential
film formed after drying in a drying oven (Universal Oven Memmert thermal analysis (DTA), and differential scanning calorimetry (DSC)
UN-55) at 50 °C for 21 h. All the tested samples were labelled with the Thermal gravimetric analysis is a method to measure the thermal
letter S (starch film), and a number corresponding to the ultrasonic characteristics of materials such as the starch based film (Abral et al.,
duration used. Thus the abbreviation S-2.5 represents starch film ul- 2018). TGA, DTG and DTA of samples were performed by using a
trasonicated for 2.5 min. thermal analysis instrument DTG-60 from Shimadzu. The samples were

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H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

Fig. 1. FESEM fracture surface photographs of the film a) before and b) after ultrasonication. Crack (i) is observed in the boundary between homogeneous (ii) and
inhomogeneous structures (iii).

Fig. 2. Opacity of the starch film after various treatments. Fig. 3. FTIR curves before and after ultrasound treatment.

weighed between 4 and 5 mg and input into the instrument which was 2.3.7. Moisture absorption and water vapor permeability
set up with a nitrogen flow rate of 50 ml/min and the heating rate of Moisture absorption (MA): Both non-sonicated and sonicated films
20 °C/min. DSC was measured using TA Instrument (Model Q20) from were dried in a drying oven (Universal Oven Memmert UN-55) until
room temperature up to 280 °C at 10 °C/min with nitrogen flow rate of constant weight then stored in a closed chamber with 99% relative
50 ml/min. The weight of each sample was 5–10 mg. humidity (RH) for 9 h. The samples were taken out and weighed on a

Table 2
Tensile properties, opacity, and crystallinity index (CI), T of O-H stretching in the peak at about 3300 cm−1 of the films before and after ultrasonication.
Sample TS (MPa)* TM (MPa)* FS (%)* CI (%) T (%)* Opacity (AUnm)*

a a a,b a,b
S-0 0.59 ± 0.21 36.96 ± 5.91 8.07 ± 3.91 12.9 9.9 ± 0.64 385.9 ± 0.73a
S-2.5 0.81 ± 0.27a 60.46 ± 9.74a 5.99 ± 2.49a 15.6 9.7 ± 0.22a 325.5 ± 0.72b
S-5 1.93 ± 0.82b 118.71 ± 50.55b 13.36 ± 2.9b 15.0 10.2 ± 0.61a,b 283.3 ± 0.15c
S-10 1.17 ± 0.17a,b 80.97 ± 9.53a,b 7.85 ± 2.05a 15.4 13.0 ± 2.29b 192.5 ± 0.06d

*Values are mean ± SD. Different letters in each column explain significant difference at 5% level of probability among sago starch films.

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H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

sonicated gel due to the kinetic energy of the jets of liquid from acoustic
cavitation scissoring the sago starch long polymer chain into shorter
lengths, thus increasing the fraction of free mobile starch molecules
(Cheng et al., 2010). Ultrasonication also breaks cross-links between
polymers, resulting in an increase in the number of mobile polymer
molecules. It also destroys the granular starch agglomerations hin-
dering mobility of the polymer chains in the gel which will result in
lowering the viscosity. Similar decreases in viscosity of the starch gel
have been observed in previous studies due to ultrasonic treatment
(Cheng et al., 2010; Iida, Tuziuti, Yasui, Towata, & Kozuka, 2008).

3.2. FESEM morphology

Fig. 1 shows the FESEM fracture surface of tensile samples before


and after ultrasonication in cross-section. The non-sonicated film
(Fig. 1a) displays a rougher surface than the sonicated film (Fig. 1b, 1c,
1d). The rough surface is attributed to the presence of partially gelati-
nized starch that impedes crack propagation. Smoother and more
homogeneous fracture surface are observed for longer ultrasonic
duration. As shown in Fig. 1a, micro and nano cracks appear at
Fig. 4. XRD patterns of the non-sonicated and sonicated films.
boundaries between the complete and incomplete gelatinized sections
(marked with i). These two sections had different molecular structures
precision balance to the nearest 0.1 mg (Kenko). Percentage of MA in resulting in a weak bonding in the boundary. As a result of this
the sample was calculated using Eq. (2) (Syafri, Kasim, Abral, & Asben, weakness, initial crack may propagate along this boundary. Further-
2017): more, where clumps of starch agglomerations occur micro and nano-
(wh − wo) sized porosities will exist between the starch agglomerations. This may
Moisture absorption (%) = x 100 result in more spaces for water molecules to diffuse. Homogeneous and
wo (2)
non-homogeneous gelatinized starch structures may experience slip-
where: page at boundary surfaces due to poor interface bonding, thus reducing
tensile properties of the film. Ultrasonication eliminates these defects
wh is final weight and wo initial weight of sample. resulting in better properties.

Water vapor permeability (WVP): Film with diameter of about 45 mm 3.3. Opacity
was stored in a desiccator at RH 50 ± 5% and 25 °C for seven days.
This film was sealed on top of a plastic bottle (45 mm diameter) con- Fig. 2 displays the absorbance curve as function of wavelength for
taining distilled water of 30 mL (100% RH). Sealing the film uses the plasticized film without and with ultrasonication for 2.5, 5 and
Vaseline for preventing the leakage of moisture through seals. The 10 min. There is a significant increase of the transparency for longer
bottle was weighed to get initial mass and stored in a closed desiccator duration (p ≤ 0.05). The S-0 film had the highest opacity
(1000 g silica gel) at 25 °C. A Kenko precision balance to the nearest (385.9 ± 0.73 AUnm) as shown in Table 2. This opacity decreases to
0.1 mg was used to weigh the bottles for each 3 h during 24 h. Average lowest value (192.5 ± 0.06 AUnm) after 10 min ultrasonication. This
WVP value was determined using the Eq. (3): lower transparency of the S-0 film is because some defects such as ag-
(dW x L) glomerations of incompletely gelatinized starch hinder light transmis-
WVP = sion (Li et al., 2015). When these are eliminated by ultrasonication,
(dt x dp x A) (3)
transmission increases. The more homogeneous and compact structures
where dW = weight loss of the plastic bottle (g), L = film thickness of the sonicated film are supported by FESEM results as shown in
(m), A = the exposed area of film sealing top of a plastic bottle (m2), Fig. 1d. This result is in agreement with a last study (Fu, Wang, Li, Wei,
dt = the time under the partial water vapor pressure gradient & Adhikari, 2011).
(dP = 2533 Pa). Three samples per treatment were tested.
3.4. FTIR spectra
2.3.8. Statistical analysis
IBM SPSS Statistics 25.0 (IBM Corporation, Chicago, USA) was used Fig. 3 displays average FTIR curve of three different locations of
to conduct statistical analysis. The effect of non-sonicated and sonicated each sago starch film for various ultrasonic treatment. Bands in range of
treatments on opacity, tensile properties, water vapor permeability, and 3500-3200, 2927, 1647 cm−1 correspond to O-H stretching, C-H
moisture absorption of the films at the 5% significance level was stretching, O-H of absorbed water, respectively (Al-Hassan & Norziah,
identified using analysis of variance (ANOVA) and P-test. The mea- 2017; Ismail & Zaaba, 2012). According to a previous study, FTIR
surements were replicated at least three times for each film tested. spectra in the range of about 3500-3200 cm−1 can be used to measure
the hydrophilicity of the biopolymer (Asrofi, Abral, Kasim, Pratoto, &
3. Results and discussions Mahardika, 2018; Matějková & Šimon, 2012). In this case, transmit-
tance (T) values in the peak at about 3300 cm−1 became higher for
3.1. Viscosity longer ultrasonic duration. For example, average T of O-H stretching for
non-sonicated film shifts from 9.9±0.64 to 13.0±2.29% after 10 min
Table 1 displays viscosity of the starch gel before and after ultra- ultrasonication (Table 2). This increasing T value can be attributed to
sonication. Two and a half minutes of ultrasonication reduces viscosity the higher hydrophobicity of the film after ultrasonication (Goyat, Ray,
dramatically from 4999 to 125 MPa s. However longer ultrasonication & Ghosh, 2011). The increasing hydrophobicity is consistent with S-10
increases viscosity that may be due to lower temperature of the gel. The film having the highest moisture resistance as shown in Fig. 6. Results
drastic decrease in viscosity can be attributed to the high mobility of the of the FTIR study are in agreement with previous work which has

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H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

Fig. 5. Curves of TG (a), DTG (b), DTA (c), and DSC (d) for all sample films. The inset of figure for glass transition (Tg) and melting temperature (Tm).

reported increasing hydrophobicity of biocomposites after ultrasonica- Hernandez et al., 2017). This result is consistent with FESEM mor-
tion (Asrofi, Abral, Kurnia, Sapuan, & Kim, 2018). phology (Fig. 1b) which showed sonicated film was more compact and
homogeneous. The fact that CI peaks after 2.5 min of sonication sug-
gests this duration is sufficient to achieve a homogeneous polymer
3.5. X-ray diffraction
structure. The slight reduction in intensity and narrowing of the three
main peaks in Fig. 4 indicates that longer sonication destroys the
Fig. 4 displays X-ray diffraction patterns for the film before and after
polymer structure (Abral, Lawrensius, Handayani, & Sugiarti, 2018).
ultrasonication. All samples show three main sharp peaks at about 18°,
19°, and 23°; a typical diffraction pattern of starch bioplastics as semi-
crystalline materials (Abral et al., 2019, p. 1800224; Duy, Rashid, & 3.6. Tensile properties
Ismail, 2012). After various ultrasonic treatments, the three main peaks
change that can be related to polymer mobility and orientation of the Average value of tensile strength (TS), tensile modulus (TM), and
polymer crystal lattice (Cheng et al., 2010; Kaith, Jindal, & Maiti, fracture strain (FS) were shown in Table 2. There was a slight increase
2009). Table 2 displays the crystallinity index (CI) of each film. CI for S- in both TS and TM and decrease in FS with ultrasonication. For ex-
0 was lowest (13%), which indicated that S-0 had the largest number of ample, TS, TM, and FS increase to 227, 221, and 66% after 5 min ul-
amorphous structures. After 2.5 min ultrasonication, CI of S-2.5 in- trasonication. These results are in contrast to the last findings (Garcia-
creased slightly to 16%. However, further ultrasonication makes in- Hernandez et al., 2017). The disappearance of defects, such as micro-
significant changes in CI of the film. The slight increase in CI may be and nano-sized cracks, ghosts (see Fig. 1a) and increased amylopectin
due to the more homogeneous polymer structure after ultrasonication in the sago starch matrix as amylopectin-rich ghosts were destroyed
(Asrofi et al., 2018a). Disappearance of ghosts releasing amylopectin or appeared to improve tensile properties (Cheng et al., 2010). However,
amylose to the matrix modifies the diffraction pattern (Garcia- film strength increases may also be a result of compaction of the

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H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

Fig. 6. MA (a) and WVP (b) of non-sonicated and sonicated film. The mean difference is significant at p ≤ 0.05. Different letters indicate significant difference among
treatment.

polymer structure resulting in a more effective resistance against ex- of the film. Thermal resistance of the film increases with a higher ul-
ternal load (Asrofi et al., 2018b). This compactness is a result of the trasonic duration. Fig. 5a shows the type of three steps of weight loss as
restructuring of the polymers in the matrix to fill micro- and nano-sized temperature increases is observed for all films. The first step of the
porosities as more active short chains are created by the ultrasonic ki- weight loss from 60 to 180 °C corresponds to evaporation of absorbed
netic energy (Abral et al., 2018). Similar results have also been reported water (Ilyas, Sapuan, & Ishak, 2018). As temperature increases to
in a previous study (Cheng et al., 2010). 180–360 °C, a second large weight loss appeared due to the volatile
decomposition of the starch film (Abral et al., 2018). As shown in
Fig. 5b, the maximum decomposition rate and the temperature of the
3.7. Thermal properties maximum decomposition for S-0 are −0.327 mg/°C, and 342.76 °C
respectively, but −0.275 mg/°C, and 357.4 °C for S-10. This result is
Fig. 5 shows effect of ultrasonication duration on thermal properties

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H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

also in agreement with DTA curve (Fig. 5c) which displays higher ac- References
tivation energy for the decomposition of S-10 in comparison to S-0, as
the second endothermic DTA peak shifts from −192.25 μV at 317.89 °C Abral, H., Anugrah, A. S., Hafizulhaq, F., Handayani, D., Sugiarti, E., & Muslimin, A. N.
for S-0 to −210.34 μV at 333.80 °C for S-10. These results confirm (2018). Effect of nanofibers fraction on properties of the starch based biocomposite
prepared in various ultrasonic powers. International Journal of Biological
thermal resistance of the film increased after ultrasonication. The more Macromolecules, 116, 1214–1221. https://doi.org/10.1016/J.IJBIOMAC.2018.05.
homogeneous structure and lower number of defects (Fig. 1d) result in 067.
a more compact structure which restricts the movement of the bio- Abral, H., Dalimunthe, M. H., Hartono, J., Efendi, R. P., Asrofi, M., Sugiarti, E., ... Kim, H.
J. (2018). Characterization of tapioca starch biopolymer composites reinforced with
plastic molecular chains which increases resistance to decomposition micro scale water hyacinth fibers. Starch Staerke, 70(7–8), 1–8. https://doi.org/10.
(Liu & Zhang, 2006). This result is also in agreement with a previous 1002/star.201700287.
study (El-Shekeil, Sapuan, Jawaid, & Al-Shuja'a, 2014). In the tem- Abral, H., Hartono, A., Hafizulhaq, F., Handayani, D., Sugiarti, E., & Pradipta, O. (2018).
Characterization of PVA/cassava starch biocomposites fabricated with and without
perature range 360–570 °C, a third weight loss represents a final de- sonication using bacterial cellulose fiber loadings. Carbohydrate Polymers, 206,
composition to ash (Abral et al., 2018). DSC curve also confirms the 593–601. https://doi.org/10.1016/j.carbpol.2018.11.054.
enhancement of the thermal resistance as shown in Fig. 5d. The glass Abral, H., Kasmianto, E., & Mastariyanto, Perdana. (2012). Mechanical properties and
microstructure of metroxylon sago fiber treated by sodium hydroxide. International
transition (Tg) and melting temperature (Tm) of sample without ulra-
Journal of Technology, 1, 16–23.
sonication was lower than that with ultasonication. For example, Tm for Abral, H., Lawrensius, V., Handayani, D., & Sugiarti, E. (2018). Preparation of nano-sized
S-0 is 187.02 °C that is lower (7%) than Tm for S-10 (200.06 °C). particles from bacterial cellulose using ultrasonication and their characterization.
Carbohydrate Polymers, 191, 161–167.
Abral, H., Putra, G. J., Asrofi, M., Park, J., & Kim, H. (2018). Effect of vibration duration
of high ultrasound applied to bio-composite while gelatinized on its properties.
3.8. Moisture absorption and water vapor permeability Ultrasonics Sonochemistry, 40, 697–702.
Abral, H., Satria, R. S., Mahardika, M., Hafizulhaq, F., Affi, J., Asrofi, M., ... Muslimin, A.
N. (2019). Comparative study of the physical and tensile properties of jicama (Pachyrhizus
Fig. 6a and 6b shows average MA and WVP before and after ultra- erosus) starch film prepared using three different methods. Starch Stärkehttps://doi.org/
sonication. Non-sonicated sago starch film displayed higher MA than 10.1002/star.201800224.
sonicated, and required a longer time (greater than 6 h) to reach steady Al-Hassan, A. A., & Norziah, M. H. (2012). Starch-gelatin edible films: Water vapor
permeability and mechanical properties as affected by plasticizers. Food
state than sonicated film. The sample that reached steady state fastest Hydrocolloids, 26(1), 108–117. https://doi.org/10.1016/j.foodhyd.2011.04.015.
was S-10, with MA of about 29.24% (a 27.39% decrease compared to S- Al-Hassan, A. A., & Norziah, M. H. (2017). Effect of transglutaminase induced cross-
0). This is because the S-0 film contains more nano and/or micro-sized linking on the properties of starch/gelatin films. Food Packaging and Shelf Life,
13(October 2016), 15–19. https://doi.org/10.1016/j.fpsl.2017.04.006.
porosities for water to diffuse into (Maneerung, Tokura, & Rujiravanit, Asrofi, M., Abral, H., Kasim, A., Pratoto, A., & Mahardika, M. (2018). Isolation of na-
2008). Sonication reduced the viscosity of the sago starch gel resulting nocellulose from water hyacinth fiber (WHF) produced via digester-sonication and its
in the more active depolymerized chains filling the porosities. Both characterization. Fibers and Polymers, 19(8), 1618–1625. https://doi.org/10.1007/
s12221-018-7953-1.
dimension and number of porosities decreased causing a decrease in
Asrofi, M., Abral, H., Kasim, A., Pratoto, A., Mahardika, M., & Hafizulhaq, F. (2018a).
diffusion of water molecules. The decrease in MA of the film is also Characterization of the sonicated yam bean starch bionanocomposites reinforced by
confirmed by the FTIR curve which shows a weaker intensity of the nanocellulose water hyacinth fiber (Whf): The effect of various fiber loading. Journal
hydrophilic functional group band at 3500-3200 cm−1 (corresponding of Engineering Science & Technology, 13(9), 2700–2715.
Asrofi, M., Abral, H., Kasim, A., Pratoto, A., Mahardika, M., & Hafizulhaq, F. (2018b).
to O-H stretching) and 1647 cm−1 (O-H of absorbed water). The en- Mechanical properties of a water hyacinth nanofiber cellulose reinforced thermo-
hancement of the moisture resistance was also confirmed in WVP curve plastic starch bionanocomposite: Effect of ultrasonic vibration during processing.
as shown in Fig. 6b. WVP value of the sample after ultrasonication is Fibers, 6(2), 40. https://doi.org/10.3390/fib6020040.
Asrofi, M., Abral, H., Kurnia, Y., Sapuan, S. M., & Kim, H. (2018d). Effect of duration of
lower than that before ultrasonication. This is because the greater sonication during gelatinization on properties of tapioca starch water hyacinth fiber
compactness in the polymer structure of the sonicated film leads to biocomposite. International Journal of Biological Macromolecules, 108, 167–176.
greater resistance to the diffusion of the water molecules (Fu et al., Cheng, W., Chen, J., Liu, D., Ye, X., & Ke, F. (2010). Impact of ultrasonic treatment on
properties of starch film-forming dispersion and the resulting films. Carbohydrate
2011; Ilyas, Sapuan, Ishak, & Zainudin, 2018). Consequently, it results Polymers, 81, 707–711.
in lower WVP values. Debet, M. R., & Gidley, M. J. (2007). Why do gelatinized starch granules not dissolve
completely? Roles for amylose, protein, and lipid in granule “ghost” integrity. Journal
of Agricultural and Food Chemistry, 55, 4752–4760.
Duy, N. Q., Rashid, A. A., & Ismail, H. (2012). Effects of filler loading and different
4. Conclusions preparation methods on properties of cassava starch/natural rubber composites.
Polymer - Plastics Technology & Engineering, 51, 938–942. https://doi.org/Doi.10.
1080/03602559.2012.679377.
Sago starch gel was sonicated for 0, 2.5, 5 or 10 min using an ul-
El-Shekeil, Y. A., Sapuan, S. M., Jawaid, M., & Al-Shuja’a, O. M. (2014). Influence of fiber
trasonic probe sonicator, then the non- and sonicated gel were treated content on mechanical, morphological and thermal properties of kenaf fibers re-
using an ultrasonic bath. Ultrasonication duration for 10 min at 600 W inforced poly(vinyl chloride)/thermoplastic polyurethane poly-blend composites.
resulted in the best properties of sago starch film including highest Materials and Design, 58, 130–135. https://doi.org/10.1016/j.matdes.2014.01.047.
Fu, Z. Q., Wang, L. J., Li, D., Wei, Q., & Adhikari, B. (2011). Effects of high-pressure
thermal resistance, the lowest water vapor permeability, the highest homogenization on the properties of starch-plasticizer dispersions and their films.
transparency, and the lowest moisture absorption. The sonicated film Carbohydrate Polymers, 86(1), 202–207. https://doi.org/10.1016/j.carbpol.2011.04.
showed a more compact and homogeneous structure, and had higher 032.
Garcia-Hernandez, A., Vernon-Carter, E. J., & Alvarez-Ramirez, J. (2017). Impact of
thermal resistance, and tensile strength than the non-sonicated film. ghosts on the mechanical, optical, and barrier properties of corn starch films. Starch
Permeability to water vapor, opacity, and water absorption capacity of Staerke, 69, 1–7.
the films significantly decreased after ultrasonication. This present Goyat, M. S., Ray, S., & Ghosh, P. K. (2011). Innovative application of ultrasonic mixing to
produce homogeneously mixed nanoparticulate-epoxy composite of improved phy-
study provides further evidence that ultrasonication could become one sical properties. Composites Part A: Applied Science and Manufacturing, 42(10),
simple, environmentally friendly process in the fabrication of sago 1421–1431.
starch film to improve its properties. Hafizulhaq, F., Abral, H., Kasim, A., Arief, S., & Affi, J. (2018). Moisture absorption and
opacity of starch-based biocomposites reinforced with cellulose fiber from beng-
koang. Fibers, 6(3), 62. https://doi.org/10.3390/fib6030062.
Iida, Y., Tuziuti, T., Yasui, K., Towata, A., & Kozuka, T. (2008). Control of viscosity in
Acknowledgment starch and polysaccharide solutions with ultrasound after gelatinization. Innovative
Food Science & Emerging Technologies, 9, 140–146.
Ilyas, R. A., Sapuan, S. M., & Ishak, M. R. (2018). Isolation and characterization of na-
Acknowledgment is addressed to Directorate General of Higher nocrystalline cellulose from sugar palm fibres (Arenga Pinnata). Carbohydrate
Education for supporting research funding with project name Polymers, 181, 1038–1051. https://doi.org/10.1016/j.carbpol.2017.11.045.
Fundamental Research (grant number 06/UN.16.17/PP.PKLN.MM/ Ilyas, R. A., Sapuan, S. M., Ishak, M. R., & Zainudin, E. S. (2018). Development and
characterization of sugar palm nanocrystalline cellulose reinforced sugar palm starch
LPPM/2019).

282
H. Abral, et al. Food Hydrocolloids 93 (2019) 276–283

bionanocomposites. Carbohydrate Polymers, 202, 186–202. https://doi.org/10.1016/ Maneerung, T., Tokura, S., & Rujiravanit, R. (2008). Impregnation of silver nanoparticles
j.carbpol.2018.09.002. into bacterial cellulose for antimicrobial wound dressing. Carbohydrate Polymers,
Ismail, Hanafi, & Zaaba, Nur Fasihah (2012). The mechanical properties, water resistance 72(1), 43–51.
and degradation behaviour of silica-filled sago starch/PVA plastic films. Journal of Matějková, Š., & Šimon, T. (2012). Application of FTIR spectroscopy for evaluation of
Elastomers and Plastics, 46(1), 96–109. https://doi.org/10.1177/0095244312462163. hydrophobic/hydrophilic organic components in arable soil. Plant Soil and
Kaith, B. S., Jindal, R., & Maiti, M. (2009). Induction of chemical and moisture resistance Environment, 58(4), 192–195.
in saccharum spontaneum L fiber through graft copolymerization with methyl me- Mohammadi Nafchi, A., Cheng, L. H., & Karim, A. A. (2011). Effects of plasticizers on
thacrylate and study of morphological changes. Journal of Applied Polymer Science, thermal properties and heat sealability of sago starch films. Food Hydrocolloids, 25(1),
113, 1781–1791. 56–60. https://doi.org/10.1016/j.foodhyd.2010.05.005.
Karim, A. A., Tie, A. P.-L., Manan, D. M. A., & Zaidul, I. S. M. (2008). Starch from the sago Nouri, L., & Mohammadi Nafchi, A. (2014). Antibacterial, mechanical, and barrier
(metroxylon sagu) palm tree properties, prospects, and challenges as a new industrial properties of sago starch film incorporated with betel leaves extract. International
source for food and other uses. Comprehensive Reviews in Food Science and Food Safety, Journal of Biological Macromolecules, 66, 254–259. https://doi.org/10.1016/j.
7(3), 215–228. https://doi.org/10.1111/j.1541-4337.2008.00042.x. ijbiomac.2014.02.044.
Li, X., Ji, N., Qiu, C., Xia, M., Xiong, L., & Sun, Q. (2015). The effect of peanut protein Segal, L., Creely, J. J., Martin, A. E., & Conrad, M. (1958). Empirical method for esti-
nanoparticles on characteristics of protein- and starch-based nanocomposite films: A mating the degree of crystallinity of native cellulose using the X-ray diffractometer.
comparative study. Industrial Crops and Products, 77, 565–574. Textile Research Journal, 786–794.
Lima, F. F., & Andrade, C. T. (2010). Effect of melt-processing and ultrasonic treatment on Syafri, E., Kasim, A., Abral, H., & Asben, A. (2017). Effect of precipitated calcium car-
physical properties of high-amylose maize starch. Ultrasonics Sonochemistry, 17(4), bonate on physical, mechanical and thermal properties of cassava starch bioplastic
637–641. composites. International Journal of Advanced Science, Engineering and Information
Liu, D., & Zhang, L. (2006). Structure and properties of soy protein plastics plasticized Technology, 7(5), 1950–1956.
with acetamide. Macromolecular Materials and Engineering, 291, 820–828. Syafri, E., Kasim, A., Abral, H., & Asben, A. (2018). Cellulose nanofibers isolation and
Mahardika, M., Abral, H., Kasim, A., Arief, S., & Asrofi, M. (2018). Production of nano- characterization from ramie using a chemical-ultrasonic treatment. Journal of Natural
cellulose from pineapple leaf fibers via high-shear homogenization and ultrasonica- Fibers. https://doi.org/10.1080/15440478.2018.1455073.
tion. Fibers, 6(2), 1–12. https://doi.org/10.3390/fib6020028.

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